Kray, 70, and two other men - builder Ronald Field, 49, and electrician Robert Gould, 39 - were charged with supplying 2kg of cocaine, valued at pounds 300,000, and conspiring with each other and persons unknown to supply 520kg of cocaine, valued at pounds 78m, said Scotland Yard.
Kray, of Limpsfield Road, Sanderstead, Surrey, and Field, of Ronson Road, Raynes Park, south-west London, were also charged with conspiracy to supply 1,000 Ecstasy tablets, valued at pounds 20,000.
The three were arrested on Wednesday night when police raided two separate addresses in south-east England.
They will appear in custody at Redbridge Magistrates Court, east London, today.
Kray - who also has a home on Spain's Costa del Sol - was arrested at a house in Crystal Palace, south London. Field and Gould, of South Park Road, Wimbledon, south London, were arrested in Grays, Essex.
They were taken to Ilford police station, north-east London for questioning.
Mr Kray's fiancee, Judy Stanley, arrived at the police station an hour before the charges were laid, with Kray's biographer, Robin McGibbon. She refused to say anything as she went into the station.