I haven't watched lots of animé; usually I just watch what my girlfriend transfers to me on IM (hahahaha... that's basically the opposite of Densha Otoko type otakus who are afraid of girls discovering their passion for animé wwww :-p).

Anyway... so, choosing from my skimpy list
I like Air for poignance.
I like Kanon for cuteness, though Kanon just has the worst character design ever.
Hmm... Love Hina, I've never watched the animé, but the manga is wonderful for laughs ^^