Biggs gained notoriety 50 years ago as one of a 12-member gang that ambushed a Royal Mail night train and made off with £2.6 million ($4.2 million), equivalent to about £40 million today. He was caught and jailed the next year.
He became the most famous of the gang after escaping from London's Wandsworth Prison in 1965, where he was serving a 30-year prison sentence, by scaling a wall with a rope ladder and spending 36 years on the run.
He used his share of the loot for plastic surgery and passage to Australia. He later fled to Brazil via Panama and Venezuela.
Living in Brazil, Biggs flaunted his freedom, was photographed partying in a policeman's helmet and in exotic locations, and in 1978 recorded a song "No One is Innocent" with the British punk band the Sex Pistols.
Tanned and sporting his white hair in a ponytail, he regularly gave interviews to British newspapers, staying in the public spotlight while in exile and revelling in his notoriety.
The Great Train Robbery became one of the most celebrated events in popular memory of the 1960s, coinciding with the Profumo affair - a sex-and-spies scandal which rocked the British establishment - and the rise of the Beatles and other working-class heroes. It spawned several films.
Biggs became a folk legend to some Britons but remained an unrepentant villain to others.
Over the years he survived a kidnap by former commandos who wanted to sell him to the highest bidder.
He was pursued across the globe by his great adversary, London police detective Jack Slipper ("Slipper of the Yard" but dodged extradition from Brazil as he had a son with a Brazilian woman.
After years of surviving by hosting barbecues for tourists and on royalties from his books, an ailing and broke Biggs finally surrendered to British police in 2001 and returned to prison but was freed in 2009 on health grounds.
His son Michael, who had been caring for him in recent years, left a message on his phone on Wednesday saying he would not be taking many calls for "obvious reasons".
'No regrets'
Biggs, who was born in south London, always said he never regretted his role in the robbery although the crime involved a violent attack on the train driver.
"It has given me a little place in history," he said in one interview. "I made good in a curious way I suppose. I became infamous."
At the 2011 launch of his autobiography "Odd Man Out: The Last Straw", Biggs said he would be remembered as a lovable rogue.
His one-time lawyer, Italian businessman Giovanni di Stefano, who had no legal qualifications and is currently serving a 14-year jail term for fraud and money laundering charges, expressed his grief at Bigg's death.
"I am glad at the very least he died a free man. His sentence was undeserved for the role that he played," Stefano said in an email to Reuters.
Biggs was last seen in public in August at a memorial service at Highgate cemetery in north London for Bruce Reynolds, the mastermind of the robbery, who died aged 81 in February.
Frail and using a wheelchair, Biggs was unable to talk after a series of strokes. He was the only one of about four remaining gang members who was well enough to make the event.
Most of the gang were caught and given prison sentences totalling more than 300 years after the robbery of the train travelling from Glasgow to London.
While the criminals struck a chord with the public as a bunch of latter-day Robin Hoods, their fame divided opinion due to the attack on the train driver.
Jack Mills was struck over the head with an iron bar during the robbery. He died seven years later and many people believed the injuries contributed to his death.
"We have always regarded Biggs as a non-entity, and a criminal, who took part in a violent robbery which resulted in the death of a train driver," said Mick Whelan, general secretary of the train drivers' union ASLEF.
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