Animal skulls, shark jaws and jewellery made from animal vertebrae have been seized at Gatwick.
Among the items found by Customs officers searching the luggage of a passenger arriving from Gambia on Friday were baboon, gibbon and green turtle skulls.
Most of the seized goods are banned from being traded internationally under the Convention in International Trade in Endangered Species.
Over the weekend, officers searched a property in Cornwall, which is owned by the passenger, and took away more articles, including leopard and tiger-skin rugs, whale teeth and tortoises. The haul would be worth tens of thousands of pounds on the black market.
A Customs spokeswoman said: "Because these animals are endangered, when bits come on the black market people will pay a limitless amount for them.
"There is a huge trade in live and dead animals by collectors throughout the world.
"Some estimates put the value of this trade almost as high as that of the illegal drugs trade."
A man has been bailed to appear at London's Snow Hill police station in six weeks' time.
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