The raid on the 50-plus mainly gold objects in the Valencian town of Villena lasted just minutes.
"The alarm at the Villena Museum went off around 5:20 am (0320 GMT)," said a spokesman for the town council, adding that by 5:24 am the thieves had already left the building.
The operation was "super-fast and super-professional", the spokesman said.
"They've taken most of the treasure," the mayor of Villena, Fulgencio Cerdán, told journalists, his voice breaking.
"We are absolutely devastated, I'm even trembling. The truth is that for those of us from Villena, this destroys us. It's part of our heritage, of our wealth," Cerdan said.
The 29 bracelets, 11 bowls, three bottles, and other miscellaneous pieces in the Treasure of Villena are kept in a small museum in the Alicante province town.
Though mainly gold, there are also pieces of silver, iron and amber, all dating back to about 1,000 BC. The treasure was discovered in 1963 by archaeologist Jose Maria Soler in a vessel sunk in a dried out riverbed in Villena.
While the treasure's historical value is incalculable, the gold alone is worth around €1.7 million ($2 million), according to the mayor.
'Through a window'
The thieves arrived in several vehicles and apparently entered the museum "through a window", according to the Spanish government's deputy representative in Alicante, Manuel Pineda.
"All security systems were activated," according to the Villena spokesman, who insisted there had been "no failure" by the museum.
Shortly before the robbery, another alarm went off at the city's sports centre and authorities were investigating whether that was a diversion created by the thieves, the spokesperson added.
Last October, thieves broke into the Louvre museum in Paris in broad daylight, escaping in less than eight minutes with jewellery worth $102 million. There have since been a series of brazen raids in institutions across Europe.
Four works "of extraordinary value" by Renaissance artist Antonello da Messina were stolen from a museum in Sicily, Italy's culture ministry said Sunday.
Two days earlier, Italian police said they had recovered paintings by Renoir, Cezanne and Matisse worth over $10.4 million which were stolen from the Magnani-Rocca Foundation museum near Parma.
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