Probably has to go to Wes Anderson's soundtracks in general. The Royal Tennenbaums and especially Rushmore were absolutely fantastic. He has a knack for great music in his films, much like other legends such as Scorsese.
In original scores, I've been partial to Air's work on The Virgin Suicides.
I would distinguish between soundtracks, and "songs from the motion picture..." compilations.
For soundtracks, I would name:
Apocalypse Now (it does contain "The End" by The Doors, but most is compositions by Walter Murch featuring Mickey Hart & The Rhythm Devils, and spoken word pieces from the film by Martin Sheen)
Star Wars
The Godfather (I and II)
Blade Runner
Midnight Express
Sorceror
Blue Velvet
Lost Highway
Twin Peaks: Fire Walk With Me
Destroy All Monsters (a Toho Studios Godzilla film - has an epic score)
Love & Death (Woody Allen film, all music by S. Prokofiev)
For "songs from the motion picture..." compilations, I would name:
The Harder They Come
Reservoir Dogs
Cooley High
Dead Presidents
SLC Punk
Trainspotting
The Big Chill
If we're going to include concert films and/or documentaries, I will add:
Stop Making Sense
The Last Waltz
Woodstock
The Decline Of Western Civilzation (1 and 2)
Scratch
Wattstax
Pacific Rim
Kung Fu Panda
Drive
Team America
True Grit
V for Vendetta
Batman Begins
The Hobbit: An Unexpected Journey
Life of Pi
Eternal Sunshine of the Spotless mind
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