Tough is a relative term. I always think of "tough" meaning the player isn't a fan of signing autographs (i.e., Mays, Griffey Jr.). But it could also mean the accessibility to that player is extremely limited or non-existent, even if they aren't necessarily bad signers (Piazza, Jeter). Mays and Tom Seaver both have medical issues that basically make them impossible to get now, although neither player can be considered rare by any stretch. Tough could also mean that the price for the player to sign is so astronomical that it would dissuade most casual fans from obtaining the signature at a signing (Koufax, Aaron).
I don't really consider any living HOFer "tough" per se, considering even the grumpiest signers are readily available on the secondary market. A guy like Mays who has not been able (or willing) to sign in recent years might be considered truly tough on a later issue card, for example, a 2019 Allen & Ginter, so the specific item could carry a premium as was previously discussed.
In terms of guys I've encountered who are just plain not friendly, my list would be, in no particular order:
Ken Griffey Jr. (though it seems he may be mellowing a bit in recent years)
Willie Mays
George Brett
Rickey Henderson
Eddie Murray
Ted Simmons
Reggie Jackson
Randy Johnson
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