The British comedian, known for his work with Ricky Gervais, is the latest name to join the cast of the X-Men spin off, reported Deadline.
Few details about Merchant's role have been released. Richard E Grant has also signed up to play a "villainous mad-scientist type" in the new instalment.
"Narcos" star Boyd Holbrook, 34, will also portray a bad guy, while franchise regular Patrick Stewart will return as X-Men leader Professor X.
"Wolverine 3" is expected to be Hugh's last outing as the character, a role he has embodied since 2000.
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