Cali was named head of the family in summer 2013, DNA Info reported at the time, taking over total control of the more than 750-person organization.
U.S. media reported that his death marked the first murder of a NY mob boss in 34 years, since the death of Paul Castellano - another Gambino family boss - by order of John Gotti.
The gunmen pulled up in a blue pickup truck outside Cali's home at about 9:20 p.m. on Wednesday evening and opened fire as the victim stood outside his Todt Hill home, police reported. After getting shot several times, Cali tried to crawl under his SUV to hide, Shea said.
Witnesses told local media of hearing at least six shots coming from outside, and seeing Cali's family members rushing outside and crying next to his body.
The Gambino family is one of the New York´s five historic Italian mafia families - along with the Genovese, Lucchese, Colombo and Bonanno families.
Gambino headed the organization until 1976, when he handed power over to his brother-in-law Paul Castellano.
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Castellano was the leader of the Gambino crime family when he was shot to death outside Sparks Steakhouse in Midtown Manhattan in 1985.
The day after Castellano's December 1985 murder, The New York Times called the Mob boss' death "highly stylized", but Giuliani dismissed such morbid romanticism. Police sources described Cali's murder as "disrespectful" because it happened right outside his family home.
Before losing his life, Cali - who usually kept a low profile - had been considered a unifying figure for the Gambino crime family. On April 6, 2009 he was released from prison.
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The body of mafia crime boss Paul Castellano lies on a stretcher outside the Sparks Steak House in NY in December 1985 after he and his bodyguards were gunned down at the direction of John Gotti, who then took over as boss.
A week ago, Persico died after serving 33 years in prison. Sylvester Zottola, 71, reportedly of the Bonanno crime family, was gunned down at a McDonald's drive thru in the Bronx last October, according to WABC. His son Salvatore had been shot three months earlier outside the family home, but survived.