Officers from Northamptonshire and Warwickshire joined Leicestershire Police for the operation.
Men aged 23 and 26 were arrested at two properties in nearby Braunstone.
Two other men, aged 31 and 35, were arrested when three properties in Beaumont Leys were searched.
The 35-year-old was charged with attempting to rob a cash-in-transit van at Bedworth, Warwickshire, on May 30 this year, and robbery of a cash-in-transit van at Rothwell, Northamptonshire, on June 3 this year.
He was due to appear at Northampton Magistrates’ Court today (Thursday 5th Sept).
All the others were released on police bail while further enquiries are carried out.