Bulger was killed in the U.S. Penitentiary Hazelton in West Virginia, a maximum security prison, where he was transferred to shortly after spending time in an Oklahoma prison, according to the Boston Herald.
Bulger had recently been moved from a prison in Florida to a transfer facility in Oklahoma City.
In 2013, Bulger was convicted of participating in 11 murders in the 1970s and 1980s and sentenced to two consecutive life sentences. They lived as Charlie and Carol Gasko in Santa Monica, in what Bulger would later describe as a "16-year honeymoon". A character in the 2006 Martin Scorsese film "The Departed" was based on Bulger.
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The death of Bulger was announced by the Federal Bureau of Prisons on Tuesday, but a cause was not provided. No other staff or inmates were harmed, said officials.
Bulger had told his attorney J.W. Carney that he regretted never marrying Greig, who abandoned her old life to join the FBI-wanted mobster in hiding.
Bulger grew up in Boston, and became the head of the feared Winter Hill Gang.
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He had been held in a high-security prison in the federal correctional complex at Coleman, Fla. He was convicted in 2013 for playing a role in 11 murders. He had a kind of Robin Hood-like image among some locals, but authorities said he would put a bullet in the brain of anyone who he even suspected of double-crossing him.
"And my thing is, as far as I'm concerned, I didn't get a fair trial", Bulger said, when he revealed he would not testify.
The gangster was arrested with girlfriend Catherine Greig, now 67.
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She may not even know that her beau, the notoriously murderous "Whitey", is dead as she's now detained in Waseca, Minnesota serving out her eight-year jail sentence.