It has always seemed to me that a good chunk of collectors seem to find the cards of HOF to be the most attractive. I believe this is a more the result of the card being artistically well done AND that it depicts a popular player that is in demand.
As others pointed out, the T206 set is littered with good looking artwork with great use of colors. Just with an available scan for example, many of these portraits would be qualify, and imagine if Lefty Leifield had a HOF career how many more admirers would rate this card near the top of the T206 heap.
Brian
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