Okay, so prepare for a VERY long reply, including all of my suggestions for Iberia! I structured it by region to make it easier to follow, and I hope this all is helpful. The work already done here is incredible. you can truly see the passion and knowledge Tinto put into making its home region!
I can see based on the location borders you used here that we worked off many of the same maps of Spanish subdivisions + some others such as the expansion of Aragon and the decline of Granada. Within each region, the additions are numbered, and the changes to a location name or borders without an addition are marked with letters. Whenever I could fine anything useful on tradegoods, I added it. I figure you can do the climate and terrain stuff far easier than me, so no direct suggestions there. Without further ado:
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Leon & Asturias
Not too many additions here, as it is already pretty dense and most major cities are represented.
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A: Sarria over Navia de Suarna
Galicia has a good density already, I wouldn't add anything. It would be great if there was a late game event that replaced Tuy with Vigo. The location names are good too, though I'd redraw the borders a bit to replace Navia de Suarna with the much more important Sarria, a key stop at Camino de Santiago
1. Grado
I understand the merging of 'Los Cinco Conejos' area into a neighbor, but it's also very odd to see a coastal city like Avilws have its location stretch so far inland. I would definitely split off Grado, which was a decently important city and Camino stop in its own right, off from Aviles, which I think also makes the size balance better, and makes Aviles a much more clearly naval location (and in fact, a nice one for say, Britain or France to take as an Iberian outpost). Seems to be a largely Livestock producing area
2. Alcanices
Zamora is rather large, and there is a clear split to its west. Alcanices is best known for the 1297 treaty there which set the Portugal-Castille border for the next centuries. It was also a fortified march centre, and had a notable Jewish minority (which mostly worked in tanneries, so maybe Livestock fits as a raw good here too)
3. Albuquerque
Albuquerque is better known for naming the future New Mexico capital, but the lords of Albuquerque were powerful nobles, and the town's population of ~7000 in 17th and 18th centuries makes it rather large for the area. If you don’t want to add a location here, I would place Albuquerque over Valencia de Alcantara in Caceres (While less important than Albuquerque, Valencia de Alcantara was still an important fortress, so I would prefer to have both)
Basque Country
I was actually somewhat disappointed by the (lack of) density here, the only regions in Iberia where that is truly the case, due to the administrative complexity and the later population boom in the region, so I have plenty of suggestions here. Adding additional locations adds more depth to the region, and makes a resurgent Navarre more powerful as well.
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1. Donostia (San Sebastian)
A very surprising omission, San Sebastian was an important city and port all throughout the period and is one of Spain's largest today. It even replaced Tolosa as the capital of the province towards the end of the game period. Most notably, however, Navarre was granted the right to use it as a port, which made it extremely important to the otherwise landlocked kingdom - there's even an argument to represent this by giving the location to Navarre
2. Bermeo
Covers the comarca of Busturia, Bermeo was the actual capital of Biscay for much of the period, making it a natural inclusion. The location also includes the later famous town of Gernika
3. Miranda de Ebro
Technically a part of Burgos rather than Alava, but it mostly takes land from the latter. This is a small location that still covers an important city and commercial center, as well as the exclave of Trevino.
4. Onati
Old city which housed the University of Onati, the only Basque university for centuries. The location also includes other important towns of Eibar (today the second largest in the province) and Mondragon/Arrasate. The trade good could be Iron to represent Eibar's famous forges, or Stone to represent the mines around Arrasate
5. Durango
Once a separate territory until being incorporated into Biscay, Durango is still the largest city in the province outside of the Bilbao metro area. It covers the southern part of Biscay, and it's mostly well known for the many New World places named after it
6. Ayala
This all leaves Vitoria even larger compared to its neighbors, so it needs a division. I went with Ayala, which was one of its major towns through the period, and contains the towns of Laudio and Amurrio, today the second and third largest in the province.
I would give Ayala and either Durango or Bermeo wine, to represent the production of the famous Basque txakoli, much like Tudela
Produces wine
This would actually allow you to split the Basque Country into three different provinces, matching the historical and modern division (with Laguardia being part of Alava as well)
Castille
Castille, like Leon, is already pretty dense compared to its number of notable cities, but there are still a few locations I would add.
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1. Mayorga
This is mostly being added to better represent Spanish administrative borders, in this case the various large exclaves of Valladolid in southeast Leon, like Mansilla represents them to the north. It was still an important strategic stronghold, and much earlier the occasional seat of power of Leonese kings. As it has a Bread museum, I'm going to guess Wheat is the main product of the area.
2. Tordesillas
Again, no need to talk much, you suggested it yourself. Famous for its colonial treaty, but it was also an important royal city for much of the game's timeline, hosting the Castillan Cortes multiple times. Famous for its Wheat production.
3. Ayllon
Splits up the large Sepulveda. Best known for the treaty that ended the Wars of the Interregnum, seems to have mostly produced Wheat, but was also an important stop during livestock migration.
4. Talamanca
Added primarily to represent the political borders (the northern salient and enclaves of Toledo of Talamanca and Uceda), Talamanca was a longtime possession of thr Archbishops of Toledo and later a royal fief, even serving as one of the capitals under Charles I. It also had a notable Sephardic community - in 1430 it had a population of 2500, 10% of which were Jewish. This, combined with its very high medieval importance, makes the inclusion make sense despite its later decline. However, if its not added, I'd make those lands a part of Alcala de Henares rather than returning them to Guadalajara or Buitrago
5. Aranjuez
Ugh, this requires a very ugly province to be viable. The case for it is obvious - a royal estate, a town so wealthy only nobles were allowed to enter, and before that the headquarters of the Order of Santiago. Seems to produce mostly Wheat and Fruit, especially Strawberries for which its famous for, so I'd probably go with Fruit. GIven how important Aranjuez is, you could also just split it off Ocana with nicer borders, ignoring the exact administrative borders here.
A: Almagro instead of Calatrava/Manzanares
Almagro was the actual capital of the Order of Calatrava, and the largest settlement in the area. I would replace Calatrava with it, or alternatively redraw the borders to replace Matanzanares with it, but I think that's not as good of a solution. Speaking of Matanzanares, given the name and the abundance of Wheat around it, changing its tradegood to Fruit would fit.
Catalonia
One of the richest regions of Spain, then as now, Catalonia has a surprising number of its important cities and county centres missing. Also includes the Kingdom of Majorca here.
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1. Prades
Perpignan is rather large, and its western parts were not part of the County of Roussillon, but formed the Vegueria of Conflent of the County of Cerdanya. The capital and most important town here was Prades.
1.5 Banyuls
This doesn't get a full number because I'm really unsure about adding it, due to the small size. Banyuls is however a very old city, and it was a part of the County of Empuries, unlike the rest of Roussillon. Well known for its Wine production. You could also instead add Ceret, representing the Vallespir Vegueria - in this case, Fruit fits way better as a trade good, as Ceret is famous for its Cherries.
A: Puigcerda instead of Llivia
Puigcerda was a much more significant place than Llivia in the beginning, being the historical capital of Cerdanya and the 6th largest city in Catalonia in 14th century. Llivia however does later gain town rights, and becomes a prominent textile center in the 19th century, but I still think Puigcerda merits the inclusion more. Regardless, it seems like the location should be owned by Majorca?
With even just one (and especially with both added), Roussillon can be its own province, consisting of Perpignan, Prades, (Banyouls), Llivia/Puigcerda and Andorra, showing the transitional zone between France and Iberia.
The various counties/comarcas just to the south of Pyrenees were small, so I understand merging them, but I'm not sure merging them into Vic and Manresa is the best way, due to terrain differences among others (they're far more mountainous). I would therefore add at least one of the following two locations (Ripoll, as it seems more important), and possibly both
2. Ripoll
Ripoll was best known for its weapons industry and metallurgy, supported by its Iron and Coal mines. This definitely helps the case for its addition, and if it's not added, I'd change Vic's tradegood to account for it.
3. Berga
Very old town (dates back to Roman times) and had its own comarca/county. Assuming Ripoll is given Iron, I would give it Coal to represent the mines in the region.
4. Montblanc
As you said you're considering adding this yourself, I won't need to really convince you much. It was the 7th largest town in Catalonia at the start of the game (and one of the five in Aragon with its own seal), with large fortifications and prominent Jewish and Muslim minorities. Seems to be primarily a Wine-producing region. Could also be given nicer, more compact inland borders based on its county borders rather than comarca ones
5. Tarrega
While this would be a somewhat small location, I believe Tarrega is definitely worth including. It had its own county and later a comarca all throughout the period. In early parts of the game timeline, it was a very important city, with a large Jewish minority - in 1348, a massacre of over 800 Jews occurred, implying a population easily in the thousands - it seems the period around the game's start was close to its peak too.
6. Inca
While Palma had municipal independence, the capital of Majorca was in Inca, so I think this addition makes sense too, and it further buffs Mallorca. Famed Wine producing region, which currently no location in the Balleares produces, despite them being a wine region with a tradition dating back to Roman times.
7. Terrassa
Covering Terrassa and Sabadell, this location would cover the inland parts of Barcelona, and while it lacks the administrative justification all the others here have, Terrassa and Sabadell were the heart of the industrial revolution in Spain. Due to their future textile manufacturies, Wool makes the most sense as a trade good, but Vegetables/Legumes also works due to the famous Sabadell onion.
Aragon
Aragon comparably needs much less additions than its two partner kingdoms, but its larger location sizes also mean that the additions are much easier to make.
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1. Monzon
Monzon was actually the capital of the comarca represented by Barbastro and Fraga here, as well as an occasional meeting site of the Aragonese Cortes and major castle. Even if it is not added, I would replace Fraga with it. Adding it however, does make the location shapes here much nicer.
2. Borja
As already suggested, Borja was a pretty important town and a major defensive fortress against Castillan invasions. It's most well known for the Borgia family that originates here however. Given the ox on its coat of arms (shared by the Borgias too), Livestock could fit as the tradegood, but so does Wine as viticulture is also mentioned as notable. The town also had a notable Jewish community.
3. Monreal del Campo
Daroca is rather large, and Monreal was a fortified town and home to one of the first holy orders in Spain. It is famous for Saffron production, as the area was one of its most important producers in Spain and Europe, so Spices could really spice up the area a bit. Arguably, even if the province isn't added, Spices would be a good tradegood for Daroca.
4. Mora (de Rubielos, known only as Mora or Mora de Aragon in this period)
Teruel and especially Cantavieja are both big, so this would help address that. Had a large castle and a custom office that collected taxes from trade with Valencia. Alongside Alcala de la Selva (another location I considered), part of the large domains of the Heredia family, later raised to a Marquisate.This seems to be a largely Livestock producing area, but also produced Wheat and Vegetables - the later might be nice to give Aragon some Vegetables/Legumes production.
5. Valderrobres
Alcaniz is also somewhat large and Valderrobres was a place of cultural transition between Aragonese and Catalan and. It was held as a personal fief by the Archbishops of Zaragoza and a seat of power for them. It seems to be a very wooded area compared to neighbors, so Lumber fits.
Valencia
Valencia is already decently dense, but it was a very rich region throughout this period, so there are many important cities left to add.
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1. Alicante
Another location you mentioned adding already, would definitely support it due to its later importance. Mentioned to be producing olives and almonds, so it should produce Fruits.
2. Alzira
Mentioned in the thread already, it was a large city, a cultural hub in Al-Andalus times and a royal city under the Aragonese. Someone mentioned Rice as a tradegood, but Alcira is primarily known for its oranges, so Fruit works very well too.
3. Borriol
While they're historical, the borders of Peniscola are awful. Splitting off the southern part would fix it, and Borriol was the most notable town there. Notably, the majority of the population was Muslim all the way until the Muslim expulsion in 1609. Primarily grows Olives and carobs, so Olives is a good tradegood.
4. Alcoy
Alcoy was an important city until it got severely punished for picking the wrong side in a civil war. It nevertheless later rebounded to become a major center of cloth industry (as well as of metallurgy and paper production). The location also includes the town of Jijona. Jijona is mostly famous for its turron, a type of nougat made from local almonds, so Fruits work here as well.
5. Gandia
Gandia is awkward to fit from an administrative and location size perspective, so I'd understand if it wasn't included. It was nevertheless a very important city for much of the period, a centre of Borgia power in Aragon and even an early university centre, declining only after the 1609 expulsion of Muslims and converts. Those Muslims operated the sugar mills that made the city rich, so Sugar is an ideal tradegood here, especially as it's otherwise not present in Valencia or the whole of Aragon.
Ayora is noted to be one of the largest honey producers in the world, so if Honey or Wax is added as a tradegood, it should definitely produce it.
Similarly, Bunol had lime and gypsum mines, so Alum or Stone make sense here, and Villar (even if replaced, see below) had kaolin, chalk and clay mines, so Clay can be the tradegood in that province.
A: Lliria over Villar del Arzobispo
Lliria seems like a much more important place, being a royal town and having recorded population since the 16th century.
Sagunt is also a notable city in this region, but I don't see a neat way to fit it without making it and Valencia too small, same with
Vilarreal right next to Castellon.
North Andalucia:
Andalucia here is divided somewhat arbitrarily, to divide it into an approximately equal number of locations added. Granada and Sevilla are in South Andalucia below.
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1. Huelma
Long location along the border with Granada, owned by the Emirate until 1438. Main productions are meat and oil, so Livestock or Olives fit
2. Alcala La Real
An important Granadan fortress taken by Castille in 1341, and further developed by them into a pretty important city (with city rights as well). Mostly known for its Olive production, but Fruit (for cherries) or Livestock would also fit as this area has many Olives, I'd go with Fruit
3. Linares (La Carolina)
La Carolina was the capital of the Nuevas Poblaciones, completely separate from the Jaen province and created to attract Catholic colonists from Central Europe to this remote area. Both were however only founded in 1767 Linares is a much older city, and is today the second most important city of the province. While it lay outside of the Nuevas Poblaciones, I'd include it in the location to make it its capital. The thing Linares is most famous for are its massive Lead mines, operating constantly since Roman times. If the province is not added, they should definitely be the raw tradegood for Baeza
4. Cazorla
Separate comarca that offers a split of the large Ubeda, it was an important border fort during the Reconquista. Grows melons, cherries and other Fruit, so Fruits fit.
If you don't want to add this many locations to Jaen, Huelma can be merged into Alcala La Real, and perhaps Cazorla not added.
5. Caravaca de la Cruz
Given all the other locations included in Murcia, I was surprised by this exclusion. Caravaca was a big pilgrimage site, and it remains so until today as one of the few Holy Cities of Catholicism. It was a stronghold of the Order of Santiago seat of a big administrative area under them, also including Yeste and Ricote ( with Yeste being a major town of over 5000 people in the 15th century). In the 16th century, Caravaca had 7000 people and was the third largest city in Murcia, after Murcia itself and Lorca. It is also a mining area, mining porphyr, jasper, Iron and limestone, so Marble, Germs, Iron and Stone are all possible - I'd probably go with Gems (or Marble) due to the uniqueness and to represent it's wealth.
6. Priego (de Cordoba)
Another location owned Granada at the start of the game. It was hotly contested, with Granada losing it for good in 1341. It was later a marquisate as well. Famous for its Olives, so they're the obvious tradegood, though Wheat is also produced.
7. Montilla
Not an administrative centre, but an important city (with city rights granted as well) nevertheless. It was the center of the powerful Aguilar lordship as well, having a population of over 13000 by the end if the game's period. Produces Olives much like the rest of the province, but it's far better known for its light sherry wines, such as the Amontillado. Would you like a cask?
The city of
Cabra is also in this area, but it would be very difficult to fit it between Lucena and Baena. I would however represent Cabra's red limestone quarries by giving one of these two locations Stone or Marble as their tradegood.
South Andalusia
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1. Zahara (de La Sierra)
Another location still owned Muslims at the start of the game. They first lost it in 1407, but managed to recapture it in 1481 - which simply gave Castille the excuse to finish Granada off. It also splits the rather large Moron location. Its famous for the chamomile gathered around it, so it would be a rare Medicaments producing location! As with other such specific tradegoods, even if Zahara is not added, I'd change Moron's tradegood to Medicaments
2. Estepa
Not the most important potential addition, but Estepa was still an important city and centre of a powerful marquisate. Estepa is mostly known for its confectionery, so Sugar could work (or Livestock, as it is made with pork fat), but it naturally produces a lot of Olives as well.
3. Tarifa
Another location you recommended yourself, Tarifa was already captured by Castille by 1337 and was their main military base in the Strait. While it lost some of its importance with the fall of Granada, it still had about 4000 inhabitants by late 16th century and its own marquisate. It's most prominent resources were Horse husbandry and tuna Fishing.
I would also redraw Gibraltar to look better when owned as a single-location outpost, for obvious reasons.
4. Alhama (de Granada)
Most well known for its hot springs, this was a favorite town of both Muslim and catholic monarchs, as well as a key fortress in Granada's defenses. It's also known for producing Legumes, especially chickpeas.
5. Motril
An important city, had about 2000 inhabitants just before it was conquered by Castille. Produced Silk and Sugar, so I'd assign one of these as the tradegood, I'd go with sugar as it became by far its most important product, especially under Spanish rule. Almunecar is redrawn and pushed into Valle de Lecrin to be more viable size-wise
6. Huascar
Covers the northeast of the current Baza location, this town switched hands multiple times during the Reconquista, being last conquered by Granada in 1324, meaning it (along with Baza) still had a Christian presence. CStille would take it again in 1434 only to lose it in 1447, before its final capital in 1488 (awful year). It had a large population, almost 600p by the mid 16th century, and it's own duchy. It later saw a large number of Basque colonists. Today it's mostly well known for being "at war" in Denmark for most of the past 200 years due to an error. It's famous for the Segureno Lamb, so Wool is the best tradegood, though Livestock, Legumes or Olives could all also fit
A: Albox over Almanzora
Albox was a large fortress, the most important one in the Almanzora River valley (also including other towns such as Purcheda), and was definitely more important than the town of Almanzora itself. The goods produced in the valley are Silk, Honey and citrus Fruits, so perhaps one of these should replace Marble.
7. Velez Blanco
Velez Blanco was the centre of a marquisate with its powerful castle. The main tradegood produced seems to be fruit
PORTUGAL:
As many people in the thread have noted, Portugal is perhaps the most in need of additional locations if it is to compete with Spain.
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A: Ourem over Chao de Couce
Perhaps the location should be Ourem over Chao de Couce? The later does seem to have been more important in the period than today, but Ourem still seems far more important.
1. Sintra
As has already been suggested, this would be a small location but a nice addition, representing Sintra and Cascais, and their palace complex, would make the wealthy heart of Portugal denser. Also home to a large Sephardic community.
Not as important, but I'd love to redraw the Lisbon/Torres Vedras border as shown to make Lisbon and Sintra only accessible from Torres Vedras - this would increase the capital's defensibility and make Torres Vedras very strategically important - and lead to great battles and sieges such as Wellington's Lines of Torres Vedras
2. Alcobaca
Leiria is a large province with a somewhat awkward shape, and Alcobaca was famed for its wine and it's monastery, the largest and most important in Portugal. The location would also include Obidos, known for its patronage by Portuguese Queens.
3. Silves
Silves was the capital of the Algarve until 1576, so it seems like a natural inclusion, despite being overshadowed by other cities of the southern coast with time. This would also mean that the four provinces of Algarve are its 4 in-period capitals!
4. Serpa
Rather simple one. Beja and Ourique are rather big, and Serpa, one of the most important Portuguese fortified towns, is missing, making for another natural inclusion. Main goods seem to be Wheat and Livestock (Cheese, for which its famous for). Copper would also fit, due to the mines in the nearby Mertola (which only began exploitation towards the end of the period however) - Mertola could also be its own location as well.
5. Estremoz
Estremoz was another important fortification towards Spain, and while Avis and Elvas aren't nearly as large, they're both very awkwardly shaped and adding Estremoz would help with that. Another good reason to add Estrdmoz is that it, Borba and Vila Viciosa are producers of famous Marble. Even if the location isn't added, at least change the raw trade good of Elvas to Marble to represent it.
6. Abrantes
A decently wealthy town and region, this mostly serves to split up Santarem. Later in the period, it was a major Silk producer.
Crato has a rather weird shape - it could be fixed by adding Proenca, but I'm not sure that's warranted.
7. Portel
The least important location I'm suggesting here, it's mostly just an option to balance the size of Evora. Seems to be a largely agricultural, Wheat producing area.
8.9.10 Braga, Mirandela, Covilha
Already explained far better than I could by Hermerico, I simply included them on the map
Now, for four less important suggestions:
11. Olivenca
The reasons are obvious - its the only permanent major change in borders between Portugal and Spanish states. On the other hand, it would be very small and not particularly rich or populous. It was however already disputed in the 13th and 17th century and a fortified town, so it is not without merits.
12. Figueira
Figueria was not particularly prominent for much of this period, but saw rapid growth towards its end. I included it as an option to further split up the rich Portuguese core and due to its later importance. Would likely produce Fish (with Fruit also being an option)
13. Valenca
Another fortress important for Portuguese defenses, unlike the southern forts it is in the already dense north, meaning there is less need and opportunity to represent it.
EDIT: oops this said Viana at first, obviously Viana is already in
14. Serta
Mostly added to fix Crato's very weird location shape, but Serta was decently important and a possession of the Hospitallers. The primary industry of the area seems to be wood, so Lumber would be the tradegood. Definitely the least important province I suggested in Portugal.
Conclusion
So that's it for this week! Again, I hope this is all helpful