Biggs, who has died aged 84, was soon caught and jailed, but his escape from a London prison and decades on the run turned him into a media sensation and something of a notorious British folk hero.
He lived for many years beyond the reach of British justice in Rio de Janeiro, where he would regale tourists and the media alike with stories about the robbery. He appeared to enjoy thumbing his nose at the British authorities and even sold T-shirts and other memorabilia about his role in the robbery.
He was free for 35 years before voluntarily returning to England in 2001 on a private jet sponsored by The Sun tabloid.
Biggs died Wednesday, daughter-in-law Veronica Biggs said. She did not provide details about the cause of death.
Most of the Great Train Robbery gang was caught and sentenced to long terms in jail. Biggs got 30 years, but 15 months into his sentence he escaped from London's Wandsworth Prison by scaling a wall with a rope ladder and jumping into a waiting furniture van.
It was the start of a life on the run that would hone his image as a cheeky rascal one step ahead of the law.
Biggs fled to France, then to Australia and Panama before arriving in Rio de Janeiro in 1970. By that time, life on the run and plastic surgery to change his appearance had eaten up most of his loot from the robbery.
In all, he spent more than 30 years in Brazil, making a living from his notoriety. For a fee, he regaled journalists and tourists with the story of the heist and offered T-shirts with the slogan "I went to Rio and met Ronnie Biggs ... honest."
Biggs recorded a song with punk band The Sex Pistols titled "No One Is Innocent," wrote a memoir called "Odd Man Out" and even promoted a home alarm system with the slogan: "Call the thief."
"It's been a screwed-up life in many respects, but a different life," he told The Associated Press in 1997. "I've never been much of a 9-to-5er."
Biggs foiled repeated attempts to force him out by deportation, extradition and even kidnapping.
British detectives tracked him down in 1974, but the lack of an extradition treaty with Brazil saved him. When Brazil's military government tried to deport him, Biggs produced a son Michael with a Brazilian woman and the law again prevented his expulsion.
In 1981, two men posing as journalists grabbed Biggs at a Rio restaurant, gagged him, stuffed him into a duffel bag and flew him to the Amazon River port of Belem. From there they sailed to Barbados, expecting to turn Biggs in and sell their story to the tabloids. But Barbados also had no extradition treaty with England and sent him back to Rio.
At a dive bar just down a winding street from the house where Biggs' lived in Rio de Janeiro, regulars fondly remembered the fugitive.
"He never talked about the heist," said Ronaldo Mendes, a 58-year-old photographer who said he often drank draft beers with Biggs.