Biggs, who was unable to speak and could barely walk after a series of strokes, was being cared for at a nursing home in north London at the time of his death, reports said.
He was part of the gang that robbed a night mail train traveling from Glasgow to London on Aug. 8, 1963, seizing 2.6 million pounds ― a record at the time and the equivalent of 46 million pounds ($75 million) today.
Sentenced to 30 years in jail in 1964, Biggs escaped from prison after just 15 months and went on the run first to Australia and then to Brazil in a globe-trotting dance with the authorities that caught the popular imagination.
In Rio he caught a lucky break ― he had a son, Michael, with a Brazilian woman which gave him immunity from extradition back to Britain.
Free from the long arm of the British law, Biggs appeared to revel in his notoriety, posing for pictures published in newspapers back home and cementing his folk hero status.
He returned to Britain voluntarily in 2001 when his physical deterioration took the fun out of the fugitive life and left him pining for home.
Biggs was immediately sent back to jail to serve the end of his sentence but was released on compassionate grounds in 2009 because of his worsening health.
He remained on parole. “The probation trust supervising him has confirmed that he has died,” a justice ministry spokeswoman told AFP.