So I don't really remember if I posted in one of these threads or not, off the top of my head I'd say both fallout 3 and fallout new vegas had great music, but if I had to choose a single game with the best soundtrack, it would be SPEC OPS: THE LINE.
https://www.youtube.com/watch?v=jZWK...E59ED5829BDA4C
(links to playlists get messed up somehow.. )