Bishop from Juice
Paris in Greek Mythology
Captain Spaulding, Otis Driftwood, and Baby Firefly from the Devil's Rejects (only because they killed with little reason)
Count Dooku (sucked as a villain)
Ultron
Kylo Ren
Green Goblin (Spiderman 2002)
Jason X
The Mandarin and the other antagonist in Iron Man 3.
Mr. Freeze character from those Joel Schumacher Batman movies.
I don't remember his name but the antagonist in Quantum of Solace 007 movie. He sucked though.
The antagonist in "In a Good Day to Die Hard" he was weak. It didn't even seem like the Die Hard movies I was use to.
***People really don't understand how a good villain can make or break a storyline, hell I'd argue the villain is more I'm important than the protagonist (hero) of the story. The best antagonist are those conflicted characters that aren't completely sinister***