If the intent is to gage true rarity, then PSA is probably not the best measure for pre-war. Regardless of PSA v. SGC v. raw, a nod has to be given first to sets like Allegheny and Alpha Engraving, which have been complete at some time in the past.
As for other sets more in the spirit, I'd think Jim B's N167 set probably tops your parameters (but I don't recall who it was graded by).
The T215 Pirate set was a near-set as memory serves when it was purchased. I'm not sure whether or not it was ever completed, but its rarity fits the direction you are heading.
E107 has been completed relatively recently for the first time, but again... not sure on the grader. That also would be right up there on the list.
I suspect that there isn't a lot of overlap on the Venn diagram of those who play the PSA registry game and those who seek pre-war, true scarcity.
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