Soul Eater: I enjoyed it, and think it's one of the few series which managed to coherently handle going off the source manga halfway through.
Gurren Lagann: I absolutely loved it the first couple of times through, especially the climactic battles. A beat weak on story in some places, but the soundtrack more than makes up for it.
FLCL: Speaking of soundtracks... Truly, this made for a good, light-hearted (except the very end) coming of age story with an unforgettable soundtrack. Ride on shooting star...
Rurouni Kenshin: There's a reason this series managed to cross cultural barriers so well. Just the right mix of drama, comedy, romance, and badass battles.