I recently bought a bunch of Ghibli films, Kiki's Delivery Service, Laputa, and Princess Mononoke.
Kiki's Delivery Service is much more for younger children than any of the others. I like the premise and the story [It's basically a bunch of shorter stories based on these Delivery's she makes as a Witch], but It could have asily branched out into a TV series, IMO.
Laputa's pretty funny, and the castle itself is really nice, very imaginitive style and chases throughout.
I haven't finished Mononoke yet, but from the looks of it it's a lot more dark. People get heads and arms cut off [No Tarintino blood splatter though, might just be the Disney cut], but it's looking very nice.
Vampire Hunter D looks really nice, haven't seen it though.
Grave of the Fireflies is pretty depressing, but very well done. About 2 kids trying to live through the second World War.
The Cowboy Bebop movie is good if you like Cowboy Bebop. It stands by itself pretty well too.
Can't think of too many else.