The suspects, which police considered dangerous, were captured inside the Mega Mall shopping centre in the posh Souissi district in an operation involving about 30 local police officers and detectives from Scotland Yard.
The Britons are suspected of involvement in the armed hold-up of a cash depot in the English county of Kent on February 22 in what is considered Britain’s biggest bank robbery.
"This theft is considered one of the most important thefts in the annals of international criminality," the Moroccan police said in a statement. They said local police had been tracking the suspects for four months.
"Due to the danger posed by the suspects, specialists in martial arts and firearms, Moroccan police had to use special techniques to neutralise them ... without posing a risk to citizens nearby at the time of the arrest," the statement said.
Police searched the Rabat residence of the four men, whose identities were not revealed.
British police said in April that they had charged six people including one woman over the robbery on the Securitas depot in Tonbridge, Kent.
More than 20 people have been arrested as part of the investigation. Only about A$50 million of the stolen money has been recovered.
Car dealer John Fowler, 60, has been charged with conspiracy to rob, three counts of kidnapping the depot manager and his family, and handling stolen goods.
Car salesman Stuart Royle, 47, unemployed Jetmir Bucpapa, 24, and
33-year-old roofer Lea Rusha, have been charged with conspiracy to rob.
Ermir Hysenaj, 27, was charged with conspiracy to commit robbery, while hairdresser Kim Shackleton, 38, was charged with handling stolen goods.
The gang's loot of A$132,123,111 was more than double the previous record amount stolen in a British cash robbery. In December 2004 a heist at the Northern Bank headquarters in Belfast netted A$66 million.
The hold-up also dwarfed other notorious raids like the 1963 "Great Train Robbery" by Ronnie Biggs, who made off with about A$6.6 million or the equivalent of A$83 million in today's money.