Personally my favorite was Final Fantasy X's soundtrack. As a soundtrack, it was original and diverse, and it also contributed much to the game's ambiance. Specific pieces I liked were the Seymour Battle Theme, Sprouting and Mount Gagazet, but ultimately the entire soundtrack was terrific, and I don't remember a single piece I didn't enjoy listening to.
I'd give special mentions to Final Fantasy IV, VI and VII as well, which also had great soundtracks.
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