Definitely The Fall. It stars Lee Pace of Pushing Daisies fame, and it is the most beautiful movie I've ever seen, artistically and plot-wise.

Whoever suggested Singing In The Rain was absolutely right.

12 Monkeys and Brazil, directed by Terry Gilliam, because everyone needs a dose of "this is so incredibly weird wtf is going on" in their lives. These movies make Donny Darko look straightforward, especially 12 Monkeys.