More than 300 officers swooped on what they described as a "very structured, professional" operation on Monday, making 20 arrests.
Police believed the gang had been targeting some of the region's most prestigious properties.
A total of 13 chateaux and two warehouses which stocked wines from several properties were targeted for robberies which have been carried out, on average, once every two weeks since June.
The thieves' modus operandi was always the same: they used stolen vehicles and sprayed bleach where they had been to ensure they left no traces.
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