Honestly, none of them. They have never done what a villain is supposed to do: Kill the protagonist. Joker, Croc, Mr. Freeze. No one has ever killed Batman... At least to my knowledge. I don't read the comics so I might have missed something, but someone needs to get the job done. I'd say the villain who could come the closest would be Catwoman. Aren't they in love or something?
For me, it's a tough call, but I'll narrow it down to three. The Joker, Killer Croc, and - one that's not listed - the Clock King. (True, he was only used a couple times, but he was pretty good for an aging accountant whose life was ruined by the advice of a friend.)
Scarecrow, both scary and quite cool when I was kid. He's the oppositte of Batman, as Batman embraces his fears the scarecrow forces his enemies to. And he was fairly awesome for his roles in Batman begins and Dark Knight.
EDIT; Like the way he attacks the mind, instead of using brute force
At the end of the Dark Knight when they're on the boat, the scarecrow is seen in a gaurds uniform which means he should have escaped
All the villians from the DC animated version and The Nolan movie verson of Batman but my favorites are Bane, the Joker, Blight(look it up), and most of all Clayface voiced by Ron Perlmen.
Joker and Harley Quinn. Love 'em... I was bummed when Harley didn't make an appearance in the Dark Knight, but I can see why they left her out. Maybe she will show up later?
I'm a fan of the Scarecrow, I was really disappointed that he didn't have a bigger role in Batman begins. Not saying Ra's Al Ghul wasn't good. My next favorite is the Riddler, he's just awesome.
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