Elaine: "Perhaps there's more to Newman than meets the eye."
Jerry: "No, there's less."
Elaine: "It's possible."
Jerry: "No, it isn't. I've looked into his eyes. He's pure evil."
I didn't know he passed. When I checked for details, I was saddened to learn that another great actress recently died- Arlene Martel. I would guess this qualifies as a villainess:
She had some great roles, and even outsmarted Spock.