Honestly, I'd have to go with New Orleans for my pick. Imagine what they could do with the whole noir theme, the architecture. The map could even be diversified by having a swampy area that's akin to the Glowing Sea in difficulty, something we could get a taste of in the upcoming Fallout: Miami mod!
If not here, I'd have to say Chicago. It's been mentioned so much, mostly in regards to the Enclave presence there. The writers could put a twist on it and frame them as the good guys, though after what we've seen them do, it could be tricky to have us emphasize with them.