Nicole at Word for Teens has a a challenge going on (with a GREAT prize!) where we pick our favorite villain and then who would cast them. She already has some good ones up so it’s actually sort of hard to think of another… but the one I’m thinking of is Devina from The Fallen Angels series by JR Ward (Covet and Crave). This is an adult series (sorry, this is what popped in my head).
Villain: Devina from The Fallen Angels Series by JR Ward (she’s a demon)
Cast: Angelina Jolie
She just is able to pull off evil and she’s absolutely beautiful. I’m not picking her by a description of Devina because I don’t remember what color hair she had or anything.