Kent Police and the Federation Against Copyright Theft (Fact) raided an address in Burnt Oak on Wednesday.
Fact described the manufacturing facility as "one of the largest counterfeit DVD operations we have managed to raid".
More than 100,000 copies were found, including current cinema release The Lion, The Witch and The Wardrobe.
Two of the three Chinese men were arrested in Burnt Oak, while the third was detained at an address in Peckham, south-east London.
DVD burners
They were taken to police stations in London and Kent for further questioning.
The crime network involved in the supply of pirate DVDs was targeted after "several months of intelligence and evidence gathering".
Kent Police's Det Insp John Biggadike said: "We are delighted to be informed by FACT that this is one of the biggest seizures to date of counterfeit goods of this type in the UK."
The haul also included computers, seven printers for producing labels and covers, 200 DVD burners and thousands of blank discs and cases.
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