There are movies that I think are better than these (the LOTR series comes to mind), but these are some of the ones that really shook my ideas of what was possible in film:
Sorcerer
Apocalpyse Now
A Clockwork Orange
Brazil
Naked Lunch
City of Lost Children
Cemetery Man
Amelie
Irreversible
Cache
Dark City
Women on the Verge of a Nervous Breakdown