Like I said in another thread, my favorite villain is Sgt Morkav in the Gary Cooper version of Beau Geste. I like him, because even though he was evil, he was an outstanding soldier and I would want him to lead me in combat.
Stannis Baratheon from "GOT" and the naked lady from "I Spit on Your Grave 2010". Stannis for being a good strategist until the writers decided to butcher his character and the sixy lady for being a good writer.
Is Hannibal Lechter (Silence of the Lambs) too easy? I really liked his intelligence. Anthony Hopkins did a wonderful job with him, too
My first choice is probably Goldfinger. I have always thought Gert Fr?be did a wonderful job of portraying Goldfinger as alternately mischievous, ambitious, charming, controlling and intelligent. I can easily imagine his Goldfinger spending years patiently and meticulously planning such a caper. It's a vivid characterization and I think it works brilliantly in the context of that movie.
Bill 'The Butcher' Cutting from Gangs of New York. Undeniably the best thing about the entire film and one of my favorites performances by Daniel Day-Lewis, a character so ruthless and violent, yet had a sense of honor.