I'm gonna pick something I shouldn't and say the English dub of Bobobo-bo Bo-bobo.
No, just kidding, though it was very funny and well done.
For anime, I haven't actually watched all of Death Note yet, I've seen the recap movies and the complete series is being shipped to me at the moment, but I haven't seen the series yet. The plot is just so well written and the characters are so interesting that it's probably the best anime I've ever seen, even if it's a bit nihilistic and doesn't really have an important moral or anything.
Also, obviously Evangelion. And Elfen Lied made me WEEP. Case Closed/Detective Conan is another good one, but it probably declines in later episodes, I've only seen the first season. Oh, and Haruhi. Call me gay but that one was entertaining as hell.
As for manga, I haven't really read anything that wasn't also turned into an anime, so I don't really have much to comment on that.
There's a lot of anime I need to watch, like Excel Saga and whatnot, but I haven't gotten around to doing it yet.