He died Saturday of cancer.
Bugliosi rose to prominence as the 35-year-old deputy district attorney assigned to try Charles Manson and several of his followers over a series of bloody 1969 murders meant to incite a race war.
The crimes, which Manson ordered to be as brutal as possible, shocked the nation. The victims were stabbed hundreds of times. One, Sharon Tate, was more than eight months pregnant.
Investigators found the words "rise," "pigs" and "helter skelter" written in blood at the crime scenes.
"As soon as I got on that case and I saw blood words, words printed in blood on a wall, immediately I told my wife, 'I don't know what the motive for these murders is,' " Bugliosi told CNN's Ted Rowlands last year. "But, I said, 'It's gonna be freaky and far out.' "
After securing death sentences for Manson and the others -- sentences commuted to life in prison when California's death sentence was abolished -- Bugliosi retired from the DA's office. He had won 105 of his 106 felony trials, including 21 murder convictions, according to his publisher.
In 1974, he published "Helter Skelter," his account of the murders and trial. The book became what publisher Simon & Schuster called "the biggest selling true crime book in publishing history."
Despite going on to a successful career as a writer after the Manson case, Bugliosi lamented to Rowlands that it was as if had had "never done anything else."
"But I'm so associated with him, I can no more disassociate myself from him than I can jump away from my own shadow," he said.
Manson, 80, remains incarcerated at Corcoran State Prison in California. He has been denied parole 12 times.
In 1991, Bugliosi scored another best-seller with "And the Sea Will Tell," his account of the double murder of a couple on a Pacific atoll. He represented one of the suspects in the case and won an acquittal.
His 2008 book on the O.J. Simpson trial, "Outrage," also reached the top of the New York Times hardcover bestsellers list, according to the publisher, making him the only true-crime writer with so many top sellers.
More recently, he had written books on the assassination of President John F. Kennedy and an indictment of President George W. Bush's invasion of Iraq.
His last book, "Divinity of Doubt: The God Question," was published in 2011.
He told Rowlands that he kept talking about Manson mostly because people kept asking him about the killings and the trial, and he said that Manson to some extent got away with murder, because his death sentence was commuted.
"He doesn't deserve to be alive. If anyone should be executed, it should be Charles Manson," Bugliosi said. "Do I go around during the daytime, 'Geez, I'm upset that he's alive'? No, I don't even think about him. I don't think about this case."