I love the Tron: Legacy soundtrack (Spotify album linked below).I also love Howard Shore's LotR and Hobbit soundtracks overall, and specifically Lord of the Rings: Return of the King by Howard Shore; and The Hobbit: Desolation of Smaug by Howard Shore. (Those Howard Shore movie soundtracks are not all metadata'd appropriately, so I can't listen to most of it here on Spotify [last.fm nightmare] Sad.)
The Wall is a 1982 British live-action/animated musical film directed by Alan Parker based on the 1979 Pink Floyd album.The Wall about a confined rocker who's driven into insanity and constructs a wall to be protected from the world around him. The screenplay was written by Pink Floyd vocalist and bassist Roger Waters. The film is highly metaphorical and is rich in symbolic imagery and sound. It features very little dialogue and is mainly driven by the music of Pink Floyd.
Control is a 2007 British-American biographical film about the life of Ian Curtis, singer of the late-1970's English post-punk band Joy Division. It is the first feature film directed by Anton Corbijn, who had worked with Joy Division as a photographer.
I can not find it on Spotify (or anywhere else for that mater), but my favorite is the soundtrack to the animated classic The Last Unicorn. The whole soundtrack was done by the band America ("Horse With No Name"), and is a beautiful album begining to end. If anyone knows where to find it in any format please let me know!