DS9: Can't say. It was the only Star Trek series I never really got into.
Voyager: Tossup between "The Doctor" and "7 of 9"
"Speaking of Thomases, I loved your recent Atrocious GM Summit column, although I think that you flatter Isiah Thomas far too much by suggesting that he is merely one of a number of atrocious GMs. The truth is that Rob Babcock and Billy King are Einstein next to him. The mess he is creating right now in New York will be studied by business school students 50 years from now alongside Enron and pets.com."
I'm gonna go off the beaten path here and say that Garak (from Deep Space Nine) is my favorite Star Trek character. You gotta love a character who once said, "I never tell the truth because I don't believe there is such a thing" and "Telling the truth is often an excuse for a lack of imagination."
Out of the five captains, I'd say Sisko is my favorite by far. He's got so many aspects to his personality. He can be gentle and diplomatic when the situation calls for it, and can be a bad-ass when he needs to be, too.
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Picard. In particular, the episode "Family." His breakdown in talking about what happened with the Borg after the physical confrontation with his brother is one of the greatest performances I've ever seen, and Patrick Stewart still managed to make it seem believable that Picard would just lose his stuff like he did.
Barclay comes a very, very close second.
TO BILL BRASKY!
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"Doubt f***s everything. Take a foundation, no matter how strong, sprinkle generously with doubt, and watch it crumble. Me? I'm unf***withable. Not this knee, not bad weather, and certainly not the many men that wish bad intentions on me can stop me. I rise up, not like a phoenix, but like the zombie corpse of Dick Murdoch. This brainbuster is for you." - C.M. Punk
I'm sure there's hundreds I could point out if I was given a list. Michaels vs Mankind is one right there that I wouldn't have thought of if I hadn't seen your list. Only one off the top of my head that I could say would be Steamboat vs Savage from WM3.