That is a pretty damned impressive list - good work. I won’t mess with it. 
Probably not quite as well known as some already mentioned, Sharky’s Machine (1981) had two villains worth mentioning (and worth seeing the movie for) in the persons of:
Victor Scorelli (Vittorio Gassman)
Billy Score (Henry Silva)
One is skin crawlingly vile and disgusting and the other is like those things that just keep coming at the hero until the hero manages to dispatch him in a convincing fashion.
“That was just business.” While it could be Moe Green was the motive, remember that Moe Green was already working Fredo.
From me I have five men and a woman.
Laurence Olivier – Marathon Man (so evil)
Walter Brennan – My Darling Clementine (so hateable)
Eduardo Ciannelli – Gunga Din (evil, hateable, charismatic)
Walter Matthau – Charade (Spoiler alert!! so likeable, so caring, then wham!!!)
James Mason – North by Northwest (charming, well spoken, evil and up front about it)
Angela Lansbury – Manchurian Candidate (the original) (soulless, manipulative, and truly evil)
John Jarratt as Mick Taylor in Wolf Creek
“It’s called making a head on a stick.”
Not mine. Jimmy Bond, all the way!
Chad from In the Company of men
An understated villain, but evil, evil, evil!
Chad talks Howard into a plot to destroy a woman ‘to get back at them for all the shit they do to us’. Chad and Howard both meet and emotionally destroy Christine, a beautiful but naive deaf woman.
They destroy Christine. Howard ends up devastated by what he has done.
In the end it is revealed that the whole time, Chad’s target for destruction was …Howard. Christine was just a means to that end. He coaxed Howard into an evil act, while taking glee in it, knowing it would destroy Howard, both personally and professionally.
This must be on the list.
I’ll second Robert Mitchum from Night of the Hunter. (awesome movie)
Robert Duvall in The Great Santini (He’s a villain, right?)
I will second Louise Fletcher as Nurse Ratched in One Flew over the Cuckoo’s Nest.
Bob Gunton as The Warden in Shawshank Redemption.
Stephen King called her the “greatest make-believe villain to come along since Hannibal Lecter” in his 2003 review of the novel. I wonder what he thought of Imelda Staunton’s performance (which it’s hard to believe didn’t receive an Oscar nomination).
James Cromwell as Captain Dudley Smith in L.A. Confidential: gentle, charming, avuncular, and pure soulless evil.
Gary Cole as Bill Lumbergh in **Office Space **
Eleanor Audley as Lady Tremayne in Cinderella.
Andy Serkis as Gollum in LOTR and the first Hobbit movie. (If we can include non-humans)
Richard White, who voiced Gaston in Disney’s Beauty and the Beast.
1.) Angel Eyes (Lee Van Cleef) The Good, the Bad, and the Ugly
2.) Richard III (Al Pacino) – the documentary Looking for Richard
3.) Norman Bates (Anthony Hopkins) – Psycho (the original)
4.) Lord Summerisle (Christopher Lee) – The Wicker Man (the original)
Anthony Perkins. Hopkins’ first film credit is from 1967, 7 years after Psycho came out. (And his first TV credit from 1965.)
I sure thought so.
Cyril Cusack (Day of The Jackal, 1984, Fahrenheit 451, 1984) was a favorite. The opposite of manical mustache-twirling, he underplayed it as a utterly corrupt old man, bored with the people he made it his duty to harm. It’s even in his George Smiley in The Spy Who Came in from the Cold.
Sian Phillips as Livia in I Claudius: like Cusack’s speech in Fahrenheit 451 explaining why books only cause trouble, her speech on how Rebuplicanism only leads to civil war and chaos shows how committed she is to villany, and anyone she has to explain it to is a stupid child. The scene where she kills Brian Blessed while nagging him is wonderful.
Olivier had a pat technique for when he played a baddie (Spartacus, Marathon Man, The Entertainer): all the muscles in his upper face slack. Completely dead expression.
Two more favorites, each of whom started as romantic leads and segued into evil old men:
Jeremy Irons (team England)
Frank Langella (team USA)
Rutger Hauer as Roy Batty in blade runner and Harvey Keitel as the lieutenant in Bad Lieutenant.
Al Pacino in “The Devils Advocate”.
“I am a Fan of MAN!”
He made virtue so lame, and sin so alluring.
FWIW, who played the Murdstones and Uriah Heep in movie versions of *David Copperfield? *
Nitpick: *** Jackal ***came out in 1973.
And TJ was played by Edward Fox. Cyril Cusack was the gunsmith.