i like iwar2. very good music. makes me feel like a tenth grader, and very circumstantially involving in the plot. also, giants: citizen kabuto had some pretty immersing comic symphony.
FF series. Although the Zeldas were pretty good. The one song that really stuck with me though was from Super Mario 64 (in the castle where you choose levels).
Oh geez I hate this question b/c I can never choose a single "best". But my top ones are:
ChronoTrigger: everything
FF6 (= FF3): Terra's Theme
MegaMan X: everything
Zelda, LttP: lightworld overworld, darkworld overworld, hyrule castle
Zelda 64: Saria's Song
StarFox (SNES): Corneria
Super Mario 64: Dire Dire Docks
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