I just watched Eden of the East, that skyrocketed into my top ten. Keeps you on the edge of your seat until the final episode, then leaves you wanting more. Glad they have the movies coming.
Other favorites include in no particular order:
Scrapped Princess (best fantasy anime I've seen yet)
Bubblegum Crisis OVA (best cyberpunk anime I've seen, also my first anime DVDs)
Full Metal Alchemist (actually just watched the first series when the second came out, now keeping up with the subs of Brotherhood on funimation.com)
Gunslinger Girl (So sad, but so awesome. The second series, so far that I've seen, doesn't live up to the first at all though)
Read or Die OVA (Fell in love with this show when I saw it crushed into a movie on CN, got the DVD the first time I saw it in a store, been meaning to check out the TV series but haven't yet)
Blood: The Last Vampire and Blood+ (best vampire anime hands down)
Neon Genesis Evangelion (like everyone else in the known anime watching universe)
Kite (may be H, but it had a sweet, tight action story and actual emotional depth, boy do you really hate the badguys by the end. Plus the fall after the bathroom fight was epic)
Nanoha (I'm not usually into Magical Girl shows, but this one had some of the best magic battling I've ever seen, particularly in A's)
The Girl Who Leapt Through Time (Entertaining, good buildup and great concept, only get's a point off because I noticed a logic mistake with the time travel)
Beyond from the Animatrix (Loved it's sort of ghost story sensibility and pretty CG layered backgrounds)
Voices of a Distant Star (Touching, amazing it was animated by 1 man)
Perfect Blue (Ausome psychological thriller, don't know what's real and what's not)
Higurashi No Naku Koro Ni (Creepy as all hell, I need to finish it still actually)
Excel Saga was awesome as it parodied everything
And as people mentioned above FLCL was trippy in an awesome way.
Melancholy of Haruhi Suzumiya is great but the Endless Eight arc is getting kindof old.
And for a couple things that fall outside of my usual watch zone but I found funny/cute:
Azu Manga Dio, K-On, and Rec. Only seen a few eps each of those so far, but always leave me smiling ^_^