Medal of Honor Allied Assault has a great soundtrack, as do a lot of the Medal of Honor games. I liked the soundtrack for Uncharted 2 quite a bit as well.
I'd really have to think about it to have a proper answer. Some I can think of now are El Shaddai: Ascension of the Metatron (most recent one I liked), Deus Ex, Final Fantasy VIII, GoldenEye, The Elder Scrolls III: Morrowind and BioShock Infinite.
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