Arkham Asylum is the only time the Mad Hatter has ever been half interesting. Or have I missed something? The fascination with fairytales and childhood actually begins to make sense with his MO.
I'd argue that he's excellent in BTAS as well. He's so devoted to Alice (or the ideal of one) that when he FINALLY finds the courage to romance her, and she turns away, he then perverts it by using his mind-control equipment to make her his slave.
Only when Batman stops him does he realise he'll
never be able to get what he wants: She'll never choose him of her own free will no matter how charming he acts, and taking her by force means he'll only ever have a doll, never the real thing. He doesn't want a mindless slave, but its the only way he'll ever get the girl. Its sad stuff, I loved what they did with him on the show, but I can't see it working in the context of the NolanGoyerverse (Burton would have done it VERY well though).
Two-face is potentially a very rich character to explore, and again I'm going to turn to BTAS for the preferred characterisation: he's already splitting BEFORE the accident, and his dark side is one he's utterly ashamed of and secretive about because, to be blunt, he's incredibly vain and egotistical already. To him, the newly inflicted half-scars mean he can no longer hide this side from himself, from his wife, or from Gotham, and since he others no longer think he's only 'good', he simply stops trying.
Wheras before his body was a timeshare, now its a vacuum in which neither personality can dominate since the coin-toss delegates both sides to chance. The personalities cancel each other out, and the end Dent is a nobody, with no moral compulsion of its own. He is both hero AND villain, but because that split takes away the abillity to make his own decisions, he can never be considered one or the other. He is genuinely insane and not just a sociopath with a gimmick.
In the animated series, his personality splits into a
third entity (the Judge) in order to fill that vacuum and attempt to overpower both personalities. Two-face is potentially one of the most interesting Batman villains, but he's hardly ever written that way.
Bane is the most directly criminal of batman's rogues. He's a steroid-using scheming south-american power-hungry egotist. The mask is just a gimmick used for intimidation and publicity purposes. He is not insane, and I cringe whenever writers have him in Arkham since he's clearly no different to any other mobster in Gotham except for the drug-taking, the mask, and the ambition. I see Bane as what Bruce could have become if he'd always been poor. They have the same raw drive, but where Batman has balanced his personal need for empowerment with his need to match his father's social conscience, Bane ONLY feels the need empower himself, to the point of being the most powerful man on earth. If Bane's parents had been better role models, Bane could well be on par with Bruce Wayne's Batman as a non-powered superhero. by the way, Does anybody know if we're ever told Bane's real name?