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JoannOf the mainstream sets I suppose Old Judge and T206's would be right up there.
But for my money, if such a thing as a complete set of T254 Old Luckey's even existed it should be the most valuable set by far, regardless of grade. In perfect grade it probably couldn't even be estimated. Just PSA 10's of Josh Adesso, Scott Marquette and Ted Behrens would have to be close to $2-3 million each. But like someone said above, it's kind of a made up question and answer, because no one has ever seen even one of these cards in close to that grade. Still though ... kind of fun to think about.
Can anyone post any of their scans from this set or of these players? Even the really beat up versions are worth 6-digits, if you can even find one.
Happy hunting. 
Joann