Clockwork Orange. I prefer the completely-synthesised version where Carlos had time to do all the music.
Rocky Horror Picture Show.
Excalibur.
Vivian Kubrick's score (as Abigail Mead) for Full Metal Jacket is phenomenal. Even the really dissonant pieces which kind of sound like someone swinging a cat into a corrugate metal fence over and over are amazing.
If you want to really talk about a soundtrack album, look no further than Apocalypse Now. This isn't just the songs and the music, but damn near the entire film, with dialogue, sound effects, everything. It's like a radio play version of the movie. I've never heard anything like it since.
Once again I agree with these, and love them, but many are originally Broadway shows made into movies, or compilations of songs that are reflective of the era of the film. They’re not necessarily original scores written for a specific movie.
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Loved the score for Jesus Christ Superstar
Can't remember all of the music from Spinal Tap but its up there with my favorite comedies.
Funny Girl and Funny Lady. My mom loved Barbra Streisand.
Hair.
West Side Story.
Picnic, Picnic, Picnic. Loved the song Picnic Morning when it segued into Moonglow.
Walk on the Wild Side.