hmmm, if it was any game it'd be one of the Guitar Heros, probably 3, but since it's ninty-only then I'd have to say... well I can't really, I love Zelda: OoT especially for the desert, guerdo valley, battle, field, and spirit temple themes. but Merio: Galaxy has some epic tracks as well. Brawl would most likely be my first choice because it has the best from every series, it has underworld from kid icarus (remixed) guerdo valley (zelda), and some excellent Fire Emblem tracks.
oh and skyman you can find a list of all brawl tracks
HERE if it wants you to regester, please do, I'm a Super Mod on that forum and we desperately need more members.