Of course, I do realise that it is very unlikely that Theramore is going to be made as big as Stormwind or any other Alliance capital. Such a thing would require a tremendous effort, while also having to seemlessly integrate these changes to the wider world.
What I do think is possible, however, is the following:
- Adding more buildings along the roads: Theramore has a lot of free space, so large parts of it could easily be filled with small buildings, as to make it feel more crowded (could also add tents filled with civilians - their presence could be explained as them fleeing from Dustwallow Marsh for safety in Theramore because of the Black Dragons). Maybe add a church as well, as it would make sense. Or a night elven embassy. Add some general clutter, as well as some trees. Aside from building in the city itself, the island's shoreline can be expanded, as to fit more stuff.
- Expanding Theramore's relevance by adding some quests. Theramore already has a reputation faction; having more quests to it feels natural. Maybe a quest that makes Alliance player visit Northwatch Hold? Or a quest that makes player visit Anchor's Edge (something like "investigate the Kul Tiran presence and find out what are they up to") that already has a few quests for the Alliance players (but no quest that leads the player there - correct me if I'm wrong). Or a quest that deals with Theramore's background as a settlement founded by Lordaeronian refugees - what if someone asks you to bring some memento from Tirisfal/Hillsbrad/Plaguelands? Or asks to find a person there (and find out that the person in question is Forsaken/Scarlet Crusade or Scourge). There also could be some quests that hint at tensions existing between Theramore and the Eastern Kindoms' Alliance members.
- Theramore's port could also be made more relevant, by establishing a naval connection to Stormwind and Auberdine (so if someone wants to get to Stormwind from Auberdine, they would need to go through Theramore port first). Menethil Harbor connection could be removed, while adding it to Stormwind, as both settlements are on the same continent (though it is probably unnecessary).