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Mark Hamill's Joker.
But, given the two, I'm probably gonna have to go with Ledger's Joker. It's a really tough call, since Bane is such an imposing villain, and honestly does way more damage to Gotham City than the Joker could ever hope to do. That whole line about how "when the chips are down, these 'civilized' people will eat each other" comes to life in Bane's Gotham, as he's able to turn half the city into a lynch mob against the other half of the city. And Bane absolutely destroyed Batman in virtually every way during their first encounter.
Buuuuuuut in terms of being an engaging and entertaining character, the Joker was just so much more interesting. He was sleazy and frightening, genuinely hilarious at points, but also really kind of pathetic. He's kind of like Tyler Durden meets the main guy from Falling Down taken to a supervillain extreme; just a bitter, spiteful man who can only derive joy from making everyone else as miserable as he is. And the fact that he's able to push Batman to such extremes, do that much damage to him on a mental and philosophical level, without the massive ninja cult and whatnot that Ra's al Ghul and Bane had, is pretty impressive.
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