If you want a great soundtrack, you should get Danny Elfman's Music for a Darkened Theater collection. It includes all of his best stuff (up to 1996) and it's on two volumes. I'm awaiting a third due to the fact that he's done a lot since '96 (e.g. A Simple Plan, Spider-Man, Red Dragon, Hulk, Sleepy Hollow, etc.). I'm mad that he still hasn't released the Theme to Army of Darkness, one of his personal bests.
Another great listen is Howard Shore's Lord of the Rings stuff. I have the piano sheet music and it's really fun to play.
There's actually a great soundtrack for Batman: Mask of the Phantasm, the best of the Batman films. It's an animated movie that sadly was tokened as a "kiddie film." If you see it you'll know that it's anything but. The score is NOT by Danny Elfman, sadly, but it sure still is kickin'.
And for those not into scores, I say the best music soundtrack is The Matrix (NOT Reloaded). I could jam to that stuff for hours.
"So I'm a heel, so what of it?"
--Renaldo the Heel, from Crimewave
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