there are a lot of good titles already mentioned here... (i finally saw Ghost in the Shell, the ending was sooo cool!!)
i still adore Akira (it's a classic, and i wasn't around for the hype so i watched it not knowing what to expect (unlike Metropolis))
and this may sound really dumb but i have a lot of love for Armitage III: Poly-matrix (yes the movie, i realize that it is quite flawed, and dubbed ::ewww::, but i can't help it, there's just something there that hooked me...)
well that was predictable and dorky... for sap i'll go w/ Grave of the Fireflies (i probably cried more during (and after) that movie than any other)
list needs something else... i should probably throw a series on there... um... or not... (thinking hurts my brain) Cowboy Beebop is probably the best series i've seen (so many good shows go bad... this one retained it's watchability throughout, kudos to you, CB!)
oh!! one more! no one's mentioned Jin-Roh! now there's a good movie! i wasn't expecting much from it going in (i'm not a big fan of the technical mission secret ops military type stuff, and that's really what it looked like...) but it completely and totally blew me away. to the point of speechlessness. (look at how much i've typed already, i don't often shut up!) it was simply amazing, highly highly reccommended.
i'll stop now.