Plus for all the undoubted brilliance of TTZ, I don't imagine that many fans can have the same sort of affection for it, the way that they do for Trek, with its regular characters, its iconic spaceship and optimistic take on humanity (though you can't deny the uniqueness of Serling's own vision).
I don't know. The fact that a fairly primitive black-and-white TV series from over fifty years ago is still airing regularly on cable and is still burned into the memories of generations of fans has to say something. I mean, I suspect that everybody on this board is familiar with most of the classic episodes and would quickly recognize any reference to some of the show's more iconic images or plots: the monster on the wing of the plane, Burgess Meredith breaking his classes, little Anthony sending people to the cornfield, "To Serve Man," etc.
As to whether it trumps TOS . . . well, it really is an apples-and-oranges comparison, given that one was an ongoing series and one was an anthology. How about we just say that they're both the crown jewels of that era's genre programming, and are of more or less equal stature?