I love Baccano. Its probably the most unique Anime out there, and so fun to watch.
Also Akikan was great for a laugh.
Needless is good too.
EDIT: As a kid, I also loved Dragonball Z and Tenchi Muyo.
The Big O was pretty interesting as well.
EDIT 2: Mangas I'd reccomend reading, but not watching are Gantz, (because its grim, VERY GRIM!!), and To Love Ru, (trust me, its veeerry embarassing to watch, (more so than akikan, but I would argue that Akikan is borderline acceptable!))
EDIT 3: The Manga that really needs to be made into an anime is Franken Fran!