As was mentioned, Goldeneye is a big one. A few others I can think of off the top of head would be Ninja Gaiden II: The Dark Sword of Chaos (the original audio, not an arrange disc) and I'd love an album for TNT: Evilution from Final Doom on the PC as well as the SNES sound for the original game.
Rockman Dash 2 would have been on the list, but we've gotten something for that game recently and since it has the best two tracks from the game on it, I'll put that one to rest. Keeping with Rockman the first Rockman World on the GB was pretty solid as well.
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