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Callisto. She had legitimate reasons for hating Xena, yet because of her choosing to be like EX became evil herself. Yet still retained the qualities that makes her largely sympathetic, even while we wish for her rampages to be stopped. Fascinatingly complex, yet still simplistically child like. No cookie cutter villain here.

Next would be....I'd say Ares, but like LK said, he's not really a true villain. Yet he's not quite an ally either and they've certainly have been adversaries.

Najara, up to the end of The Convert, was a kick butt villain as well. Like Callisto, she's a bit of a mirror of Xena, which makes for some really interesting complexities. What is/isn't good or for the greater good and who gets to make those decisions. Fascinating.

For that matter, the Horde in The Price were pretty interesting villains - largely because things turned out to not be quite as simple as Xena and the Athenian army first thought and they turned out to not really be 'villainous' at all.