Officers from the National Crime Agency (NCA) found items including a tiger's head, monkey skulls, reptiles and stuffed birds of prey during raids in Newton Abbot, Devon.
The man, 40, was arrested on suspicion of breaking laws protecting endangered species and bailed until September.
It follows the seizure by the UK Border Force of a chameleon preserved in formaldehyde at Heathrow.
The reptile, found last month, had been shipped from the United States. As a controlled species, there were strict rules in place to prevent its illegal importation.
The discovery led NCA officers, supported by UK Border Force officers, to a Newton Abbot business address on Thursday.
Dawn Cartwright, from the NCA's Border Policing Command, said: "Unregulated imports or exports of rare species can have a devastating impact on their survival, which is why the law around moving them is so strict and we take potential breaches of that law so seriously.
"Working with Border Force and our law enforcement partners, we will continue to target the international criminal trade in endangered species."
A man has been arrested after a haul of exotic animal parts was seized.