Well in the OT I love both Rat King and Leatherhead and Irma is amazing and I love every episode she is featured heavily in.
2k3, Bishop was actually my favorite villain from the whole series, Hun does a great job at getting you to hate him and I love the Ancient One, both for the family aspect of his character and because he is a rip off of some many Kung Fu films I watched and loved.
I think each one of these characters impacted the story in big, yet very different ways!