It's close between U2 and TLOU1.
Overall I'd still go with Uncharted 2, I just find it really fun to play and to this day it's still one of the few games that truly nails the cinematic experience. The big setpiece moments found a great balance between cool scripted stuff while still giving the player enough freedom to feel like they are taking part in the action instead of just walking in a straight line as cool shit happens around them, which is something that a lot of other games, including newer ones like Uncharted 4, struggle with.
TLOU1 has the more emotionally engaging story and the fighting has a more tense and impactful feeling to it, but I found the overall gameplay loop and presentation slightly less engaging.