Police have so far seized £14 million in cash after swooping on a safe depository in Edgware on Monday, suspected of being used by criminals to store assets.
A gun, counterfeit passports, works of art believed to be from the Renaissance period and other valuable items have also been uncovered in the unprecedented operation involving 300 officers.
The depository, in Manor Park Crescent, was one of three run by private firm Safe Deposit Centres that was searched.
Two people have been arrested on suspicion of money laundering and are believed to be directors of the firm.
Leslie Sieff, 60, was arrested in Finchley Road, Hampstead, and Jacqueline Swan, 44, was arrested in Park Street, Marble Arch.
They were bailed to return to a central London police station in early September.
Two men, aged 47 and 53, were arrested for obstruction in Park Road, Marble Arch, but have been released without charge.
The firm's two other branches were raided in Hampstead and Park Lane as well as an office and three houses.
The investigation was the first of this scale the Metropolitan Police has ever conducted against suspected criminals using this type of secure storage.
The three vaults contain an estimated 7,000 boxes ranging in size from A4 drawers to walk-in cupboards. Police suspect up to 90 per cent of them might contain criminal assets.
People who are concerned about their property stored at the depositories can call 0800 030 4613.
Anyone with information relevant to the investigation is asked to contact Crimestoppers on 0800 555 111.
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