When it comes to as a person that would likely be zhao. He literally killed the moon out of pride and ambition.
However as an antagonist zhao was excellent. in fact I would almost put him on par with azula (yes I would) when it comes to antagonist criteria. While he is undercut a bit in the second half, he presents a great threat for the gaang and the narrative, he has a lot of power, the will and desire to use it and he is competent. Also he presents a threat to both sides of our main characters including iroh and zuko