Officers with the Guardia Civil confiscated 126 ivory carvings of various sizes, many featuring Asian-style designs, from a trading company in the eastern region of Valencia, the force said in a statement.
They also seized a 1.77-metre (5.8-foot) tusk weighing 22 kilogrammes (48.5 pounds), believed to date back to the 19th century.
Authorities said the items lacked proper documentation.
An analysis confirmed the ivory came from African and Asian elephants, both of which are protected under the Convention on International Trade in Endangered Species of Wild Fauna and Flora (CITES).
One woman was arrested and four other individuals were placed under investigation.
The World Wildlife Fund estimates that around 20,000 African elephants are illegally killed each year for their ivory tusks, despite international trade bans.
Ivory -- sometimes called "white gold" -- has historically been one of the world's most sought-after commodities, used in jewellery, weaponry, musical instruments and ornamental carvings.
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