Alec Baldwin - narrator in The Royal Tenenbaums. Alec Baldwin should narrate everything.
Brendon Small - Home Movies and Metalocalypse.
H. Jon Benjamin - everything he has done, ever. Dr. Katz. Home Movies, Lucy, Daughter of the Devil, Archer. Bob's Burger's wasn't terrible, but I wasn't in love in love with it.
Richard Epcar - Kenshin, Samurai Champloo and Witch Hunter Robin.
Robin Williams - definitely a favorite VA.
Ron Howard - Arrested Development
Steve Blum, indeed - Spike and Shishio from Kenshin.

I wish Dave Foley would voice more characters, because I love him and playing a robot for Fallout just isn't enough for me.