Best soundtracks in Games...

GTA: San Andreas
Borderlands
Quake 4 (MCC Landing)(Main Theme IMO)
Assassin's Creed 2
Crysis 2 (Main Theme)
The Elder Scrolls IV: Oblivion
The Elder Scrolls V: Skyrim
Need for Speed: Underground 2
Need for Speed: The Run (Menu Theme)
Need for Speed: Most Wanted
Need for Speed: Underground
Fallout 3 (Intro)
 
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The Elder Scrolls (especially Oblivion and Skyrim) have awesome soundtracks. Hmmm...not really sure if this counts though, but San Andreas' radio stations were spot on and perfect for the game and gave it that '90s atmosphere.
 
Best song ever in a game?

Portal 1 end credits! BEST EVER!

Oh, I also remember Homeworld having some pretty awesome background music.
 
There are so many. Mostly Yoko Shimomura's work are good, her orchestrate release drammatica is exceptional.
Most memorable would be Final Fantasy OST because there are so many of them released.
 
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