My top five are the same as TrueTears. Weird coincidence, I know. The order is a bit different though. I'd remove the first season of Clannad and replace it with the original FMA. Oh yeah, I also have mixed feelings about Code Geass R2 so I'd probably remove that. The rest I agree with. Gurren Lagann is epic and awesome as is Death Note. Clannad:AS is super sad and emotional and Brotherhood is just great action, interesting plot and fantastic characters. Oh yeah, the original season of Code Geass was great, full of twists and over the topness that kept everyone coming back.
For movies I'd put in Howl's Moving Castle, the Disappearance of Haruhi and Spirited Away. The Haruhi movie is way better than the TV series, since it's really well animated and actually has a really interesting plot. I was killing to find out what happened next.