The whole Silent Hill series, Akira Yamaoka does absolutely brilliant job in the music department, fits to the games really well and creates a really creepy atmosphere.
I really liked the soundtrack from Mass Effect 2. It succeeds in setting the mood for all situations. I can also get behind the FFX suggestion, which is also great.
The BlazBlue series. A unique character theme for each character and a couple of Vs. themes, alongside the JAM Project-esque Bang Install, lyric'd versions of some themes and console opening songs sung by KOTOKO. Might sound overwhelmingly Japanese, but that's just because you haven't listened to the sheer quality of the perfectly themed music. Gluttony Fang, Marionette Purple, Memory of Tears... The whole damn soundtrack could stand on its own as outstanding without the game.
Tony Hawk's Pro Skater 2. Every time I hear "Guerrilla Radio" I automatically think of skateboarding because of that game. Some songs from Papa Roach and Powerman 5000 don't hurt either.
God of War 2. Best main menu theme of the series. I still hum it to this day.
Like the OP said, Uncharted 2 because the main theme makes really sharpens you up for some treasure hunting.
And I totally agree on Morrowind's soundtrack. Better than Oblivion's, I thought. That could just be the nostalgia talking though...
My contribution:
I think a great many videogame soundtracks are really excellent. For me there isn't a best one. I guess I'm just easily pleased. But one game which I didn't expect to have marvellous music and really took me by surprise, was Mirror's Edge.
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