Serial Experiments Lain
Key The Metal Idol
Now And Then, Here And There
My Neighbor Totoro
Neon Genesis Evangelion
Requiem From The Darkness
Elfen Lied (It's still growing on me, actually)
some episodes of Cowboy Bebop
The second half of Trigun (the first is borderline unwatchable)
Anything by Leiji Matsumoto (Galaxy Express 999, Captain Harlock, etc.)
Ghost In The Shell
the first volume of Ergo Proxy is awesome, and I'd be surprised if the rest of the series didn't follow suit
Paprika (the new movie by Satoshi Kon, check it out)
And other stuff. I know I've forgotten things (you see how I almost forgot FLCL there? Foolish!) but most of the critical stuff is in there.
It's grime time.