I like The Dorf's first portrayal in Ocarina of Time. The concept of a brash, sadistic, tyrannical young prince with delusions of grandeur is so compelling - especially given how easily he manages to rise and fall (though not through any lack of effort on Link's part). This dude grew up the only guy among a harem of thieves, ordained to be their sovereign since birth, and raised by a couple of keese-shat crazy old witches. There is just no way this poor kid was going to end up as anything other than utterly evil. His arrogance and smooth confidence makes for a compelling villain.
Second favorite? Twilight Princess. Here we have an older Ganon who got his arse handed to him in ways this poor megalomaniac just couldn't possibly accept. Cynicism has clearly taken over. Gone is the brash arrogance and smooth confidence of his youth. TP Dorf is a madman tempered by defeat. In a way Ganondorf's defeat only made him stronger. And by stronger I mean royally pissed off. TP Dorf is very straight forward. This dude is just pure full on unbridled psychopathic rage. No frills. Just seething hate and anger. Terrifying.
Honorable mention? Wind Waker Ganon. This guy's awfully sympathetic. I mean, heck, if you read between the lines Link and especially Daphnes come off as jerks. The narrative of WW is so vague and haphazard it doesn't even really bother to explain what Ganon was trying to do exactly. In a sense he's a guy who admires Hyrule as much as Daphnes. I'm certain the Dorf wouldn't have been a benevolent ruler, but we see him here as a sad defeated man on his last desperate bid to claim the land he fought for repeatedly. Kinda pathetic really. Aspects of Ganon's portrayal here don't really jive with the rest of the series and even its own game. For instance, Ganon is rarely referred to as Ganondorf and we never see aspects of his bestial nature despite his monstrous form being depicted as the force that called for the flooding of Hyrule in the first place. But I chalk these complications up to WW's slipshod execution overall. Still, WW managed to portray the Dorf in a way you could almost understand and sympathize with.
Lease favorite? Demise. If by "least favorite" you mean "strongly desire to viciously eradicate all historical evidence of and pretend it never happened." Demise is flat out insulting. To Ganon's character and the whole TLoZ mythos.