A truly memorable villain is a study in complexity. It's not enough to twirl a mustache and demand the rent or don a hockey mask and swing an axe. Not for me at least.
Ten you'll l-o-v-e to hate:
Henry Fonda/Frank in Once Upon a Time in the West -Just so you know he's really bad to the bone, he shoots a kid, in the BACK.
Rutger Hauer/John Ryder in The Hitcher- A bored sociopath thumbs a ride.
Dennis Hopper/Frank Booth in Blue Velvet- An inhalant addicted sadomasochist looks for romance.
Kathy Bates/Annie Wilkes in Misery- An avid reader who doesn't care for the ending of a series. Instead of a well worded letter, she opts to kidnap and terrorize the writer for revisions.
Javier Bardem/Anton Chigurh in No Country for Old Men- He's a hired killer, that occasionally offers a victim a 50/50 chance at freedom on a coin toss, just for fun.
Ian McDiarmid/ Supreme Chancellor Palpatine in Star Wars: Return of the Jedi- Darth Vader is considered black hearted, and this is his master. His sarcasm is especially cruel.
Arnold Schwarzenegger/Series 800 in The Terminator- Before he returned as a good guy/protector, who asked questions and cried, Arnold was fantastic as the relentless, lacking-any-social-skills Terminator.
Angela Lansbury/Mrs. Iselin in The Manchurian Candidate- Ambitious, calculating, devious AND a Mom! When she plants a long kiss on the lips of her hapless son, it is perfectly creepy.
Joseph Cotten/Uncle Charlie in Shadow of a Doubt- When he returns to his small hometown and says to his niece that was named after him, "The world's a hell. What does it matter what happens in it?" you know bad things are coming.
Bette Davis/Baby Jane Hudson in What Ever Happened to Baby Jane? - Some think that this film is campy but I think Bette Davis is truly menacing as Jane. When her wheelchair bound sister (played by Joan Crawford)complains, "You wouldn't be able to do these awful things to me if I weren't still in this chair." Jane responds, "But you are Blanche! You are in that chair!" Brrrrr!
I didn't include the obvious choices: Margaret Hamilton as the Wicked Witch or Anthony Hopkins as Hannibal Lecter or Anthony Perkins as Norman Bates who top any Baddie list.