Based on my own opinion, I'd say Aquaman.
Objectively tho, it's a different case. Aquaman only has Black Manta and Ocean Master as recurring villains, and while I love them, it's not the general consensus. Same goes for Wonder Woman (Cheetah, Circe, Ares), Iron Man (The Mandarin, Iron Monger), Captain America (Red Skull, Zemo, Crossbones) and Hulk (Abomination, Leader). Cool and the gang on their own, but not striking in quality and quantity.
Out of the ones left, I think Thor has the shittiest end of the stick. He has a couple of cool villains and a lot of them at that, but tbh, most are extremely mediocre outside of some of the better stories. Plus, Aaron ruined a lot of Thor villains like Mangog, Malekith etc.
So with Superman, Flash and Green Lantern left I'd say Superman. Not because I think his villains are the best, but because of the lack of originality for the other two. The Flash has like, speedster villains and the Rogues, who are original villains, but they are all he has. Literally every notable Green Lantern villain belongs to a Lantern Corps, which is an original concept on it's own, but I feel like the Corps should have other cool villains not tied to the emotional spectrum.
Superman has a wide variety of villains such as Brainiac, Doomsday, Lex Luthor, General Zod, Parasite, Cyborg Superman etc. I feel like each of them is fleshed out and all of them are different sorts of characters.
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