Chrono trigger - Top notch stuff
Final Fantasy series - I especially liked FF4 (2 in the USA) FF6 (3 in the USA) and FF7
Starfox 64's soundtrack reminds me of Dvorak's music, which is a GOOD THING.
Ocarina of time had some really nice tunes.
Super Smash Bros. Melee had a lot of good remixes .. Zelda II temple and Fountain of Dreams come to mind
Metroid Prime had some really nice songs -- Tallon Overworld, Magmoor, and Ridley boss theme come to mind. The latter two were also in Super Metroid.
The Mega Man series of games have some really good songs (and some not so good songs too)
Top Gear (the original, also known as Top Racer)'s four songs for the tracks were good
The Sonic games for Genesis had some
very cool music. Tunes like Toxic Caves in Spinball were very nice.
Sonic CD had great music, primarily because it was true CD audio.