If we're talking beyond the now standard 2.5" x 3.5" baseball card, any Topps card prior to 1957 would qualify, no? In that case, I might go with the 1953 Bowman Pee Wee Reese (hey, it makes it by 1/4", haha!)
If we're talking bigger than a baseball card, which is what I think hockeyhockey is referring to, one of these would probably be my pick.
 
Of course, the N142 cabinets are fantastic, too.
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Building these sets: T206, 1953 Bowman Color, 1975 Topps.
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