Metal Gear Solid 1,3 and 4 (i'm not really too experienced with 2) Just brilliant atmosphere defining music, it has it's own style and Harry Gregson-Williams is a damn genius! if the Metal Gear movie ever gets going, he has t do the soundtrack.
I liked Mass Effect and Bioshock, but a game that kind of surprised me at how much I liked the soundtrack was Digital Devil Saga. I was glad I bought the special edition that came with the soundtrack. Fantastic use of guitar for just about everything! It was pretty damned fantastic for me.
The Witcher.
Epic Soundtrack. Especially in....well, everywhere...combat music, ambient music, but my favourite was at the very end, credits. Very powerful. Great thing is, you can go through the game files and pull out the .OGG files, convert them to Mp3 and listen to them anywhere.
Some of the games, that come to mind, where the sound-track was very fitting/enjoyable are.. Demon's Souls, JSR, Timesplitters 3, Red Alert 3, and godhand, for just being strangely catchy.
As... er... "interesting" as recent titles have been, I've never been able to badmouth the soundtrack to any Sonic game - with the possible exception of Unleashed, which I haven't played and so plead ignorance. Sonic CD (the European/Japanese version) is a particular favourite of mine.
Same goes for anything involving Nobuo Uematsu.
Not to mention Jet Set Radio and its sequel, a big pile of Nintendo titles (Brawl has a decent selection) and the Metal Gear series.
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