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Vader
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Shark
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Hannibal
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Imotep
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Velociraptors and Nazis, give 'em both a half-vote.
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Scrappy Doo. The moment he came online you couldn’t help but hate him. Plus he wasn’t a puppy at all. He had a glandular problem.
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Dorothy from the Wizard of Oz. Elpheba was a biproduct of political conspiracy and was framed. Evil Dorothy killed the first person she happened upon and then teamed up with three complete strangers in order to kill again. Wicked Dorothy indeed!
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Voltan (Jack Palance’s character in Hawk the Slayer). There were so many things wickedly wrong with him from the fact that he looked at least 20 years older than his aging father whom he killed to his relentless pursuits of Hawk for the use of his birthright for ornery purposes to the fact that Jack Palance fell mightily when he took this role.
Great movie for its pure cheesiness factor. -
FranknFurter (Rocky Horror) He had all the best lines, all the best songs, and he was twisted enough to take in two true blue American kids and turn them into sexbots. Janet the slut and Brad the bisexual. I wish I were a sweet transvestite from the planet Transexual as well. Boomchicka Boomchicka Boomchicka Boom. I see you quiver in antici…
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Ashram the dark knight (Record of the Lodoss war). This is the first real 3 dimensional villain I have seen. It isn’t exactly a movie but oh well. Ashram has believable motivation (rather than to simply be evil) and is very easily related to once you learn his motivation. It makes sense and all villains should be as fleshed out as he is.
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Keyser Soze, because he’s evil itself and just so smooth.
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Darth Vader, for being a powerful giant who breathes while he talks. For years, the sound of Vader breathing meant “bad guy”.
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Michael Myers, the original unstoppable killing machine. Created slasher horror.
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Dracula. I doubt any character has been more widely used as a vehicle for villainy.
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Dawg Brown, from the biggest money-loser of all time, Cutthroat Island. Frank Langella plays Dawg perfectly, as a crazed pirate captain who’ll slit your throat as soon as look at ya.
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Hannibal Lecter
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Darth Vader.
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Jack Wilson (Jack Palance) in Shane. He’s not just evil. He’s Eeeeeviiilllll.
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Michael Myers.
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Bruce Dern’s character in The Cowboys. (Good call, plnnr.)
Oh, now, he’s only done three Austen Powers movies!
[Yes, I know.]
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Keyser Soze. It helps that I’m a fan of the actor.
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Hannibal Lecter. Also already mentioned. Masterful.
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Zorg from The Fifth Element.
I can’t believe no one has mentioned Zorg. He’s evil and avaricious. He blows up anyone working under him that he finds stupid. He knows and admits he’s a monster. He’s got the wickedest haircut ever. Okay, “Mr. Shadow” was the ‘big bad’, but Zorg was human. You could try to relate to the guy. -
Bela Lugosi’s Dracula.
“I never drink … wine.”
“To die… To be really dead… That must be glorious.”
“There are far worse things … awaiting man, than death.”
“The children of th night … what music they make!”
I mean, honestly, how can this character not be in the top five, not to mention in the top fifty? -
The Alien from Alien.
A couple already covered…
Tony Montana - Scarface
Nurse Ratchet - One Flew over the Cuckoo’s Nest
and
Reverend Harry Powell - The Night of the Hunter.
A chilling charismatic predator. The tattoo speach is one of the all time great movie scenes.
Harry Lime - The Third Man
A man totally without a conscience.
Mr. Blonde - Resevoir Dogs
“I don’t give a good fuck what you know or don’t know, I’m going to torture you anyway.”
No mention of Plankton
“F is for fire that burns down the whole town.
U is for uranium, BOMBS!
N is for no survivors…”
- How many of you have played musical instruments before?
Do instruments of torture count?
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HAL, 2001 : A Space Odyssey
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Nurse Ratched, One Flew Over the Cuckoo’s Nest - (Please, try to spell her name right, I’m afraid we might upset her.)
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Harry Lime, The Third Man - the friend you wish you never knew.
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Franz Becker (Peter Lorre’s character), M
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Darth Vader, Star Wars - Did he scare you as much as he scared me?
Hon. mentions : Lady Kaede (Ran), Evil (Time Bandits), Jaws (metalmouthed man of James Bond), Jaws (the shark).
Why did the only two people I wanted to mention get taken already…curse my tardiness.
Anyway, futile second votes go to Bricktop from Snatch and Mr. Blonde from Reservoir Dogs.
And I’ll thorw in some votes for Zed and Maynard from Pulp Fiction, they’re pretty evil.
The Sheriff of Nottingham, Alan Rickman, from Robin Hood: Prince of Thieves. I am a big Robin Hood fan, but the sheriff is the only reason to watch this movie. I had to pick him over Hans Gruber, because I think he’s just more psycho in this role.
The Terminator. “It can’t be bargained with! It can’t be reasoned with! It doesn’t feel pity, or remorse, or fear. And it absolutely will not stop, ever, until you are dead!”
Magneto from X2. Well, probably from X-Men as well, but moreso from X2.
After all he came thisclose to wiping out humanity.
Belloq from Raiders of the Lost Ark. He’s suave and charming enough to make people forget that he has a black heart.
The Bug from Men in Black. “Imagine a giant cockroach, with unlimited strength, a massive inferiority complex, and a real short temper, is tear-assing around Manhattan in a brand-new Edgar suit. That sound like fun to you?” Normal cockroaches are evil enough already, who needs one that’s about 8 feet tall.
And even worse, he’s French. 
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Hannibal Lecter - Just terrifying the first time I saw the film. Trumps Vader and others because I prefer my villains human. Pure evil.
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Jake Heke - From the New Zealand film Once Were Warriors. Truly the scariest man on the planet. Played by Temuera Morrison in one of the best performances I have seen in a long time. Wins the award for the film character I would least want to offend.
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Bruno Anthony - From Strangers on a Train. Just plain creepy. Check on the tennis scene where he remains still as the spectators heads move back and forth watching the action. Hitchcock’s greatest villian, Psycho be damned.
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Harry Powell - Night of the Hunter. A classic film with Mitchum’s stunning performance.
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Nurse Ratched - Louise Fletcher deserved a better career than she had. She outshone the rest of a great cast in Cuckoo’s Nest.
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Darth Vader from Star Wars and Empire Strikes Back - for the reasons stated above.
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Bernie Birnbaum from Miller’s Crossing - The Dane was menacing, but in the end it turns out he was right all along. Johnny Caspar was psycho, but basically had a ethical code, however twisted. But the Schmatta Kid is a smarmy, unctious, two-timing, back-stabbing, snivelling little bastard with absolutely no redeeming values. Brilliant performance by John Tuturro.
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Count Orlok from Nosferatu (the original) - the movie itself is comical nowadays, but that image of the vampire is horrifying on its own. I’ll never forget it.
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Bill Lumbergh from Office Space - great smarmy performance from Gary Cole, and the sex scene is one of the funniest scenes of any movie. One of the best villains because he’s one of those completely frustrating, noxious people we’re all more likely to have to deal with than vampires and Imperial overloads.
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Wicked Witch of the West from The Wizard of Oz - as others have explained. Flying monkeys can’t be beat.
I didn’t pick Hannibal Lecter, even though Silence of the Lambs is one of my favorite movies ever, because Jame Gumb is the real villain in that story. Lecter is just “supporting villain.”
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Mr. Potter from * It’s a Wonderful Life* - He’s just a “warped, frustrated, old man”.
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The villain from the movie Something Wicked This Way Comes - I can remember being freaked out by this villain, and intimidated especially in the parade scene.
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Hans Gruber from * Die Hard* - “Now I have a machine gun. HO HO HO!!”
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The Terminator from * Terminator* - That scene where he jumps on the hood of the car, and punches through the windsheild, especially sticks out for me.
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The Admiral from * Star Wars* - He controlled Darth Vader!!!
No votes yet for Mrs. Iselin in The Manchurian Candidate? That was one cold, cold bitch.
Hannibal Lecter, from Silence of The Lambs, as well as The Red Dragon, was the first to come to mind when I read the title of the thread.
Hans Gruber was the second. I love Alan Rickman!
Annie WilkesShudder! The scariest thing about her is that psycho fan/murderers are all too plausible!
Surprised no one has mentioned Pennywise from It. With lines like “They taste so much better when they’re scared!” to, “Down here, we aaalllll float!”, all done in the tres-creepy voice of Tim Curry, yikes!
The Six-Fingered Man from The Princess Bride (he can share the title with Prince Humperdinck, if you’d like). To kill aman in front of his young son, slash the son, and leave. . .well, I loved the movie, and believe that he is the best comic villain ever!
Max Cady - Cape Fear (De Niro, remake)
Crafty evil. Personal. Sexual. Avenging.
Jake LaMotta - Raging Bull
Cruelty fueled by insecurity. Pathetic.
Nurse Ratched - One Flew Over the Cuckoo’s Nest
A classic evil authority figure.
Alex Forrest - Fatal Attraction
Suddenly, the cute girl in the next cublicle doesn’t seem so tempting, does she?
Annie Wilkes - Misery
But she was nice sometimes. 
OK, I’ll play.
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Amon Goeth from Schindler’s List: I can’t believe no one has mentioned him yet. Knocks all other screen villains into touch, simply 'cause he really was that bad.
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The Wicked Witch of the West from The Wizard of Oz: she’ll get you, my prettys, and your little dogs too.
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The Toecutter from Mad Max: would just as soon kill you as look at you; in fact, would much rather kill you than look at you.
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Begby from Trainspotting: poster boy for Drunken Racist Louts, Ltd.
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Godzilla: Ohhh, Ohhh, there goes Tokyo…
While none of these equal Hannibal, Darth, et al, I didn’t just want to repeat them again:
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Karen (Nadine) and Manu from Baise Moi
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Derek (Edward Norton) in American History X
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Alex, A Clockwork Orange
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Mr. Blonde, Reservoir Dogs
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Ian McKellen, Apt Pupil
Honourable Mention: Sam Rockwell in The Green Mile