1 Joker (Heath Ledger) - The Dark Knight
"Some men aren't looking for anything logical, like money. They can't be bought, bullied, reasoned, or negotiated with. Some men just want to watch the world burn."
-Alfred Pennyworth
2 Loki (Tom Hiddleston) - Marvel Cinematic Universe
Loki Laufeyson, or Loki Odinson, is a fictional character appearing in the American comic books published by Marvel Comics. He is the adoptive brother and archenemy of Thor, and is known as the "God of Mischief". In the Marvel Cinematic Universe, the character has been portrayed by Tom Hiddleston. Loki (Tom Hiddleston) can't be as good as heath ledger's joker but is still the second best superhero movie villan, also hiddleston's performance is one of the best in the superhero movies after ledger, rdj and hemsworth. This is just my opinion though.
3 Magneto (Ian McKellan) - X-Men series
Magneto is a fictional character appearing in American comic books published by Marvel Comics, commonly in association with the X-Men.
4 Doctor Octopus (Alfred Molina) - Spider-Man 2
5 General Zod (Terrence Stamp) - Superman I & II
Wait a minute never mind thought this was man of steel one. this is the one I prefer.
I voted for the Man of Steel Zod, not the one the name says '-'
6 Thanos (Josh Brolin) - Avengers: Infinity War
This villain had 6 years of build up and the wait proved why he is the best villain hands down.
7 Bane (Tom Hardy) - The Dark Knight Rises
Bane is a fictional supervillain appearing in American comic books published by DC Comics, commonly as an adversary of the superhero Batman.
8 Joker (Jack Nicholson) - Batman (1989)
9 Green Goblin (Willem Dafoe) - Sam Raimi's Spider-Man Trilogy
The Green Goblin is the alias of several fictional supervillains appearing in American comic books published by Marvel Comics, mostly those starring Spider-Man. The character first appeared in The Amazing Spider-Man #14, and since then he has become one of the characters most famous villains. He was the main antagonist in the 2002 movie Spider-Man, in which he was portrayed by William Dafoe. He was awesome, and let's face it guys, he couldn't avoid being over the top, no one can play green goblin without being over the top, it's just naturally gonna happen
10 Ultron (James Spader) - Avengers: Age of Ultron
The Contenders
11 William Stryker (Brian Cox) - X2
12 Ra's al Ghul (Liam Neeson) - Batman Begins
Ra's al Ghul is a fictional supervillain appearing in American comic books published by DC Comics, commonly as an adversary of the superhero Batman.
13 General Zod (Michael Shannon) - Man of Steel
14 Mr. Glass (Samuel L. Jackson) - Unbreakable
15 The Penguin (Danny DeVito) - Batman Returns
The Penguin is a fictional supervillain appearing in American comic books published by DC Comics, commonly as an adversary of the superhero Batman.
16 Sandman (Thomas Haden Church) - Spider-Man 3
The Sandman first appeared in The Amazing Spider-Man #4 (Sept. 1963), created by writer Stan Lee and artist Steve Ditko as an adversary of Spider-Man. The character returned in The Amazing Spider-Man #18 and #19, and was soon depicted in other comics, such as The Incredible Hulk and The Fantastic Four. He is sulky and didn't need to be in the movie.