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Akira.
Uhhhm, Oskar und Leni I suppose, although I have never seen the movie, though I hear it's quite rubbish, I just love Penguin Café Orchestra. Same goes with Koyaanisqatsi, that's a good soundtrack too. I saw This is England and loved it but I cannot remember the soundtrack at all. I went through a huge Yann Tiersen phase after Amélie, so I'll have to agree on that one.
Dazed and Confused
Blade Runner
Donnie Darko
Aliens
Just to name a few.
For the sheer hilarity of the soundtrack, has to be fallout 3.
Shaft
The Fountain's easily my favourite. I think the music fits the film perfectly.
Moon, also by Clint Mansell, is good. I'll always have a soft spot for Crouching Tiger, Hidden Dragon's soundtrack as well.
I love Rocky Horror, though I've got to give it to Cowboy Bebop yo. <3
I do like the tracks for pick of Destiny, even if I disliked the movie.
Disney films that Alan Menken worked on also have very good soundtracks.
I have so many that I can't list them all here.