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Anthony N.Up in the running (besides those mentioned above)....
Any '61 Dice Game, any '70 Cloth Sticker, '60 Fleer #80's Grove, Tinker and Collins.
Not quite as scarce but still really, really tough are '58 Hires Test with tabs.
I'm sure there are a few dozen other cards that rank up there. The Leaf Paige is tough, but not by any means impossible.
Most overrated scarcity, IMO? '54 Bowman Ted Williams.