Dark City. Its one of the greatest sci fi films ever made, but was so strange under promoted that it is not very well known. It has such an amazing story, great images and some theams like the Matrix but is so much better then that film.
Animation wise I think Time Masters and Gandahar(light years) are great. They might not be my favorite animated films but they are just so awesome and weird. René Laloux is a master of his craft.
I don't know if this can even be found anymore, but if you ever get a chance get a copy of The Star Wars Holiday Special. It's a made for tv movie from the 70's. The basic story is Chewbacca is trying to get home for Life Day. Pretty much the first 20 minutes or so is all in Wookie. This movie has to be the most amazingly bad wonderful thing I've ever seen. The average person is usually only able to stand the first 45 minutes. I love inflicting the Special on the unsuspecting lol.
Malice in Wonderland (it's a trip... Also? Hatter), The Ramen Girl (soooo much better than the dvd covers make you think), Sunshine (Cillian Murphy and Chris Evans... mmmhmmm), The Quest for Camelot (Cary Elwes as a voice actor? yes please), Cat's Don't Dance (come on guys! Animated dancing, singing cats!), The Island (...I've got a thing for men from the UK apparently...), The Fall (artistically stunning), Ink (bizarre and hard to follow but pretty awesome all the same) and Inkheart (which no one wants to admit to seeing/liking, but I'll sing its praises up and down for giving us long haired and shirtless Paul Bettany).