I base it by personality, and brains really. I love the Hulk, Iron Man, and Thor because of their comedic moments, but Black Widow was just more appealing by her smarts (Outsmarting Loki was the funniest serious moment) and by her style when fighting. That, and she's hot as hell xD
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Lol, that was probably my third favorite moment 
My second favorite was the Thor/Black Widow moment on the ship, where he says:
"He may beyond reason, but Loki is of Asgard. And he is my brother."
"He killed 80 people in 2 days."
"He's adopted."
And my all time favorite was when the Hulk just owned the crap out of Loki by slamming him around the ground xD
My second favorite was the Thor/Black Widow moment on the ship, where he says:
"He may beyond reason, but Loki is of Asgard. And he is my brother."
"He killed 80 people in 2 days."
"He's adopted."
And my all time favorite was when the Hulk just owned the crap out of Loki by slamming him around the ground xD
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His expression made my day lol xD