For a nice 2D anime look you can get FANTASTIC results with Ockhams Z-Flatten (z-toon) python script in the freestuff here!!  It works amazingly well and gives everything a nice dark cartoony outline and even works while animating!

Of course you can always try the material shaders route but in my opinion the z-toon method looks more authentic and me being as avid an anime watcher as I am (I watch tons of anime Cowboy Bebop & Ergo Proxy are my favorites!! ) I'm more than satisfied with z-tooning!!

Gerard

The GR00VY GH0ULIE!

You are pure, you are snow
We are the useless sluts that they mould
Rock n roll is our epiphany
Culture, alienation, boredom and despair