The latest person charged is 24-year-old Jetmir Bucpapa who is accused of conspiracy to commit robbery at the Securitas depot in the town of Tonbridge, in Kent, southeast England, last Wednesday.
He was set to appear before magistrates in Maidstone Friday morning GMT.
The charge came after two men and a woman became the first to appear before magistrates earlier on Thursday.
Car dealer John Fowler, 60, was charged with conspiracy to rob the depot, kidnapping the facility’s manager, wife and nine-year-old son, who were held at gunpoint, and handling stolen goods.
Fowler, reportedly a multi-millionaire wheeler-dealer figure, owns the sprawling farm estate in Staplehurst, Kent, which police officers have combed for evidence in recent days in their hunt for the missing loot.
Car dealer Stuart Royle, 47, of Maidstone, was charged with conspiracy to rob, and his self-employed hairdresser girlfriend Kim Shackleton, 38, was jointly charged together with Fowler with handling stolen goods.
That charge relates to steel cages that were used to hold the stolen money, later found ditched in a field.
The three suspects were remanded in custody to appear again at Maidstone Crown Court on March 13.
A total of 14 people have so far been arrested by police in their attempt to catch the gang, who pulled off a robbery which more than doubled the previous British heist record.
The previous record was 26.5 million pounds (A$62.08 million), stolen from a Belfast bank in December 2004.
Police insiders told London’s Evening Standard newspaper that the raiders left behind a trail of clues.
A source told the daily: “At first it was assumed that because of the scale of the operation, we were dealing with experienced robbers.
“It is increasingly apparent that those involved did not fit that profile at all. This gang made basic mistakes.”