+1 to FMA: Brotherhood.  It is one of my absolute favourite animes of all time.
Also +1 to Cowboy Bebop.  If you liked Samurai Champloo, you'll more than likely enjoy Bebop.  They were made by the same guy.

I also really enjoyed Knights of Sidonia.  There are two seasons out currently, both complete.  It kept me gripped for both series and I just loved every second.  Netflix is the best legit way to watch it, but I'm sure it'd be on either of the sites you mentioned.

Psycho Pass is another really good one.  It's got a very compelling setting and storyline and is nice and dark.

Neon Genesis Evangelion is another favourite of mine, but I'll admit that it gets pretty difficult to follow.  But as far as it's visual appeal and it's soundtrack, it's legendary.