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Ghetsis is probably my favourite because he actually feels sociopathic, devolving into totally unhinged by the end of his arc in BW2. He also feels the most evil because his plans involves a human element; N. None of the other leaders have the same impact because when you hear passing mention of Team [___] "abusing pokemon" you never really get to see much of it and it's never expanded on, so you can't relate to it or get an idea of what's really happening or why it's bad, you're just told it's bad and expected to go along with the narrative. Ghetsis however, he's abusing a person; a child he stole away and groomed into a tool for his own selfish means.
The speech at the end of Black and White where his mask finally slips and he absolutely berates N for failing him is so brutal it actually stings. Not to mention he goes as far as attempting to kill the protagonist with Kyurem, something none of the other leaders ever dare to attempt, and when his alternate timeline counterpart arrives in Ultra Sun/Moon, he doesn't back down and accept defeat when he's beaten like all the others, he smacks Lillie to the ground and threatens to kill her if you don't surrender.
He doesn't get a moment of resolution where he changes his tune like Archie or Maxie, he doesn't silently slip away and vanish like Giovanni, Lusamine or Cyrus, he goes down swinging: a deranged and cruel monster to the very end.
