Narses of the Belisarius novels is pretty villainous and ruthless, willing to betray anyone, by his own admission. Oh, yes, he did help the good guys win in the end because it was best for him - but they still made a point of giving him chests of treasure and a one way trip to China. Despite that, he clearly loves Ajatasutra in a father-and-son sort of way.
Hardly heady lit, but there was a series of bestselling historical “bodice ripper” novels and an accompanying miniseries about a Georgia plantation called Beulah Land. The villain was Roscoe Elk who begins as the racially ambiguous overseer of Beulah Land and becomes its nemesis and the richest man of color (what that color is exactly not even Roscoe knows- he just knows he’s free and dark skinned- possibly mulatto, possibly Indian) in the south. He’s a despicable, murdering, socipathic character, but late in his life he becomes a very affectionate grandfather towards his grandson, Roscoe III; everyone is surprised at his tenderness towards the boy (who becomes a philanthropical “anti-Roscoe” in later novels).
Angus Thermopyle from The Gap series was a very very evil man who took a lot of risks and made some huge sacrifices out of love.
Jaws in Moonraker
Khan.
The eponymous Flashman was an utter bastard, but in his own admittedly perverse {and decidedly non-monogamous} way, he genuinely loved his dimwitted but redoubtable wife Elspeth, and not just carnally. Rather touchingly, they lived into their nineties together.
One of my pet odd theories is that in James Cameron’s Titanic, Billy Zane’s character really does love Rose quite a bit; he just has no idea how to handle her. If the ship hadn’t sunk, I could see him forcing her into a mold she was never meant to fit, making her miserable, and destroying the very things he loves about her. If you wear your tinfoil hat just so, he’s a rather tragic figure.
OK, stop laughing!
The villain in The Bad Sleep Well, who really loves and dotes on his handicapped daughter.
Hannibal Lecter loved his sister Mischa. To lesser degrees he loved his aunt (name eludes me- Japanese lady married to his uncle in Paris) and Starling.
Boris and Natasha seemed fond of each other when they weren’t making 'Beeg troe-bil for Mooze and Squoreel.
Dr. Horrible, of course- though he’s more of a villain-in-training than a true evil mastermind.
Sulla from the Masters of Rome book series truly loved his son, Young Sulla.
I think it was implied in one story, at least, that Lex Luthor had a thing for Lois Lane. And Namor definitely has a thing for Sue Richards (he was a villain who did his Heel Face Turn really early on).
There’s this guy on the Straight Dope boards who has a complex multipoint plan to take over the world and become it’s overlord, [thread=481902]dividing the management of it into multiple satrapies run by deserving dopers
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He also introduced his wife to the Boards.
Is this the kind of thing you’re after, M’lord?
The Mayor’s sincere love for Faith occurred to me when I read the title of the thread! Of course, you used him in the OP.
Spike & Drusilla were together for a long time. We hoped those crazy kids could make it! Even at the end, Spike admitted he was Love’s Bitch.
Also on Buffy, I think it’s clear that villainous Spike loved Drusilla very sincerely.
(edit) and now I see that Bridget beat me to this observation by one minute.
Doesn’t the Joker occasionally seem to love Harlequin?
I might be remembering this wrong.
I actually agree with this theory. Remember, Cal realized a small moment of redemption when he gave up a waiting seat on that lifeboat in order to make sure that Rose made it off the ship safely. “Oh, damn it all to hell…” I actually felt sorry for, and maybe even admired him a little in that moment. Not to mention he’s also the funniest character in the movie: “Picasso? He won’t amount to a thing. Mark my words!”
Scorpius from the Farscape series. I can’t quite put my finger on the flavor of love he has for his second-in-command, Braka (though it probably involves bondage), but they’re definitely joined at the hip.
I was coming in to mention Harley Quinn. I don’t know that she really counts as a villain. And yeah, Joker loves Harley. Otherwise, she’d be dead. Of course, a lot of that is because everything she does is wrapped up in him, so it’s massive ego-boo, but no one said it had to be healthy love.
How about Black Adam and Isis?
Oh, and Mumm-ra loves Ma-mutt. Most of the time.
From the Vincent Price fanclub-
Dr. Anton Phibes- his wife Victoria & perhaps his android Vulnavia,
Edward Lionheart- his daughter Edwina (Diana Rigg) in THEATRE OF BLOOD.