24 Once Upon a Time villains ranked worst to best
Nimue
Merlin was such a tragic character, and I think having Nimue be the first Dark One was a compelling twist to the Dark One origin story. And so cruel to Merlin! His love starts off so sweet at first, but slowly lets darkness overtake her, eventually creating the first evil entity that drives the whole show. Nimue was sadly too far gone, but she made for an interesting antagonist.
Dark Swan
I really wish the Dark Swan could rank higher on my list because this was such a unique idea in taking the Savior and making her a Dark One. But for some reason, Emma as the Dark One was always so stoic. This character could have been funner. I don't know, the storyline and the Dark Swan overall didn't end up as intriguing to me as I was hoping for.
King Arthur
Another usual hero but turned villain in Once Upon a Time's version is King Arthur. Getting obsessed about succeeding in something can make a person go crazy and do things they woulnd't. And that's what happend to the King of Camelot. He was intent, dangerously so, to make Excalibur whole. But in doing so, he used the Sands of Avalon on his wife Guinevere. This was completely wrong of course. But I think in King Arthur we got a guy who goes off the hinges which admittedly is fun to see.
Isaac/Author
One weasel-y character that can be considered a villain is Isaac, the previous author before Henry. He's slippery like an eel and knows how to play the heroes, which I think he did really well. He's selfish and finds ways to get what he wants. Though Isaac doesn't have magic except for the powers of the Author, he causes much trouble to our heroes. Even sending them into the Heroes and Villains storybook that's an alternate universe.