MW2 definitely only because that's one of the greatest soundtracks of any game. But I feel since it's Hans Zimmer, one of the greatest movie composers out there for films, it's kind of cheap. I don't really care though. All of the songs in the game are very very good. But I think if I had to say which was the best of them all, it has to be the Boneyard Flyby song.
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Personally, I think The Official Dead Space Soundtrack is. There are a lot though. The Darkness, Chronicles of Riddick: Escape from Butcher Bay, etc.
One soundtrack that I haven't seen mentioned in this thread yet is Forza Motorsport 3's. In addition to licensed tracks, the game has a lot of original pieces for its menu music, and they're all very soothing.
Hell March 3? Personally I believe that Hell March 2 is superior. I've also put up another RA2 soundtrack and some more from Emperor Battle for Dune because seriously the soundtrack for this game needs to be more known about.
A lot of people hated the Quake soundtrack when the game came out since it wasn't the hard ass metal industrial stuff they expected. But I think it's brilliant and creepy as all get out.
That said, here is the theme from Relentless: Twinsen's Adventure. That version comes off the CD version. Beautiful. The rest of the music is just as good.
Enternal Sonata, don't like many Japanese RPG's but I sort of fell in love with this one and one of the main reasons was it's stunning soundtrack. Being a Frederic Chopin fan as well helps I guess. Stunning soundtrack throughout.
@TheFreeMan: The World Ends with You had a awesome soundtrack, a number of stunners. Speaking of which I'd love to see more of that series for the 3DS.
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