Really depends on how the rest of season two goes down. Ra's al Ghul seems like the most obvious choice, considering how much he has been hinted at this season. But perhaps they will hold off on him for a while.
Merlyn might be a bit redundant as as a season-long villain again. I'd like to see him around again as a recurring nemesis for Team Arrow, but not to the extent that he was the big-baddie of season one.
Perhaps Ravager will take over as the main antagonist next season? Or maybe Blood? Waller - and by extension: the Suicide Squad - is another option.
And, of course, Arrow could always introduce a new villain. I think it might be fun to see some more super powered antagonists next season. Deathstroke is plenty fun with his super-strength and his healing capabilities. But I want to see some villains with crazier abilities. Maybe introduce a new Count Vertigo, one closer to his interpretation in comics, who comes to Starling from Vlativa because the original "Count" had been providing his country with the drug and his death resulted in Vertigo losing a significant amount of power over his people, or something. I think Arrow could have fun using a more traditional interpretation.
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