Apparently the largest atmospheric test done in Nevada was 74kT (https://en.wikipedia.org/wiki/Plumbbob_Hood)
It's kinda hard to imagine why on earth you'd ever build a warhead larger than 100kT. At that point it's just destruction for the sake of destruction, not to win a war, but to ensure that everyone loses... Well, that is the point of MAD, but it just seems reckless and inhuman.