Isabela OK, lbr, Isabela's in a pretty grey area as far as that goes to begin with.
The only reason she's a heroine is because she teams up with one.
But Dread Pirate Isabela is the terror and scourge of all Thedas. No morals whatsoever. Does whatever brings her a profit and to hell with anything else.
She is cold and ruthless and brutal and as likely to shank you as look at you.
Kallian ...oh, sweet Kallian. She's not so sweet anymore. No, she is pissed as hell and out for revenge.
Human male nobles and templars are her favorite targets, and she takes all healing skill and instead of knowing how to make a body work right? She knows exactly how to make it self-destruct.
She becomes everything people are taught to fear about both mages and elves.
Ingrid Probably started fine, but... yeah, she'd go Red Templar. She was just following orders, and now she's corrupted.
Edgar as a villain is... honestly kinda scary. He's subtle, manipulative and traps you long before you realize it. He's everything you would expect from a Dark Fairy.
And once he has you... you are his plaything. Don't expect a quick, clean death. Oh no. He will toy with you until you bore him.
..and then you'll probably be tortured to death.
Varda as a villain... probably paired up with the other brother--Melkor instead of Manwe. Whatever light she gives is cold and harsh. She is cold and distant to the people of Arda.
She delights in the darkness as much as he does, though.
Amroth and Celebrian are probably not all that different than Galadriel if she had taken the One Ring. Beautiful, charismatic... all would love them and despair.
Imladris becomes a trap--a honeyed lure into unimaginable darkness. And Lothlorien's gold masks the corruption it holds.
Piper becomes everything she ordinarily hates about the Aphrodite cabin: manipulative and catty. Lures people in and then stabs them in the back.
She takes whatever she wants. She makes people her thralls on a whim with her charmspeak.
Di as a villain...Probably dabbled in the wrong kind of witchcraft and got corrupted or possessed or merged with whatever the fuck thing is after her, IDK;.
Nerdanel as a villainess joins forces with her infamous husband and sons, and she's the craftiest one of them all. Feanor acts too rashly--she tempers him, plays the long game.
At first she seems reasonable, but really, she's using that time to delve deep into a person's psyche, learn their weaknesses and then exploit them without mercy.
Melkor doesn't stand a chance, but her hands are also burned by the Silmarils, which then sends her into a spiral of fury and grief because it robs her of her gift for art.
Myth kids are just their assholish sides all the time without any redeeming charm.