As another self-admitted "centering freak", it's interesting to see everyone's take on which cards are the toughest to find centered, and of course it's fun to see all the cards. Thanks for allowing some postwar cards on this side of the forum, Leon.
I do not own one, and I'm surprised this one hasn't been mentioned, but the 1952 Topps Eddie Mathews card is notoriously off center, if not miscut. This example was posted back in 2015 on the BST for just over $5K. Like a cheapskate, I sent the seller a slightly lower offer while someone else bought the card for asking price in the meantime. I am still kicking myself over this one, and I even saved a scan to remind myself about the opportunity lost. Talk about a cardboard unicorn:
Here's a few examples that were already mentioned, all picked up over the years with an attention to centering:
The Clemente RC isn't that tough