Hmm. I'd say it's either Bill Cipher or the Lich. I suppose this comes down to if you want a entertainingly evil villain or a terrifying villain. Don't get me wrong, Bill is scary, but he's also funny and more deliciously evil, whereas The Lich is just outright scary and has almost no funny moments, which is the point of his character. Personally, I prefer The Lich since I love a scary villain in a lighthearted show, but I could also definitely see preferring Bill.