The arrests took place on Sunday and were made following a description given after the robbery, of both the suspects and the vehicles.
One of the assailants is believed to have been carrying a gun during the robbery.
In related news, Algarve GNR officers arrested two men, also on Sunday, on suspicion of having committed unrelated acts of domestic violence in the areas of Albufeira and Lagoa.
According to a statement from the GNR, the first suspect was arrested in Albufeira as part of an investigation into crimes of domestic violence being conducted by the Public Prosecutor.
Searches on the suspect’s house and vehicle turned up a .22 magnum gun and 53 rounds of ammunition.
The suspect detained in Lagoa was arrested on a warrant also as part of an ongoing investigation into domestic violence.
Both arrests were carried out by the Portimão branch of the Special Victims Investigation Bureau (NIAVE), and both men were fitted with ankle tags and forbidden from making any form of contact with the victims.