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.