I hope I'm not stepping on any toes, and if I am.....too bad. But to me, actually, the best soundtrack.....Windwaker. I know that sounds wierd, probably one of the most shunned Zelda games in the franchise (and ironically, later the future innovator for pretty well all the ensuing handhelds) but the thing that really saved it for me, after the graphics, and hours of sailing, and the even more hours of searching for maps and getting 8 stinkin' shards of the triforce, was the soundtrack. I could turn on my gamecube and listen to that intro music over and over again. The soundtrack for that game was pretty epic.
TP came close, but no, windwaker takes it for me