Absconded prisoner and convicted armed robber Michael Wheatley - aka the "Skull Cracker" - was arrested in east London police confirmed on Wednesday.
The arrest came hours after Wheatley allegedly robbed a building society in Surrey.
Kent Police said in a statement: "Kent Police, in partnership with officers from the Metropolitan Police Service, have today arrested two men in east London on suspicion of conspiracy to commit armed robbery.
"On May 3, Kent Police began a search for Michael Wheatley, who had failed to return to HMP Standford Hill after being released on temporary licence.
"At 2pm on May 7, two men, aged 55 and 53, were arrested in the Tower Hamlets area and are now in police custody. The 55-year-old man was also arrested on suspicion of being unlawfully at large."
DCI Ann Lisseman from Kent Police said: "We are no longer looking for Michael Wheatley. We would like to thank our colleagues at Metropolitan Police Service, Surrey Police, and the public for their assistance with our enquiries."
Jodie Aston, 30, who works in a hair and beauty salon just yards from the building society, said police officers told her they knew who the suspect was.
She told the Press Association: "They came in and said the man that robbed the bank was the man that escaped from the open prison and it happened at 10.20am.
"We heard nothing until someone came in and told us. It's quite scary to think we were so close. It could have been in here."
Barmaid Chloe Theobald, 26, said she was alerted to the incident when she was having lunch with her manager.
She said: "The police said to my boss 'We think it's the Skull Cracker and he's been sighted in Sunbury'. It's quite scary. It's not something that happens every day that there's a man on the loose.
Wheatley, who was given 13 life sentences at the Old Bailey in 2002, earned his notorious nickname after pistol-whipping victims - including a 73-year-old woman - during the raids.
Prosecutors said he returned to a life of crime after a relationship with a woman he met while in custody turned sour, and she spent his money and ran up debt.
At the Old Bailey hearing, lawyers revealed that when asked his occupation by a custody officer, he replied: "Armed robber."
The 55-year-old raided 13 building societies and banks over 10 months in 2001 and 2002 while on parole from a 27-year sentence for other robberies.
Wheatley admitted 13 charges of robbery and 13 of possessing an imitation firearm - a blank firing semi-automatic pistol - in October 2002. He is one of more than 1,200 open prison inmates serving an indeterminate sentence.
He had gone on the run twice in the past and each time staged a series of violent robberies before being caught and re-jailed.