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Alec Baldwin
He was a major movie star and goes seamlessly between tv and major movies. He's great on SNL and was a huge part of 30 Rock's success. And he still does big movies like the Mission Impossible series.
As some lagniappe to this, Alec Baldwin was originally considered for the role of Nucky Thompson on Boardwalk Empire. From tidbits from Mark Wahlberg and Scorsese contract issues and prior commitments derailed it.
I wish there was an alternate timeline where I could of seen that series.
Steve Buscemi is a great actor, deserves to be on this list as well for weaving between great TV and great film, but Baldwin would of been a perfect anchor for that show. Probably heightened it above the slightly above average place it ultimately fell.