Cali, thought to have headed the family since 2015, suffered "multiple gunshot wounds to the torso" in front of his home on Staten Island on Wednesday evening, police said.
Cali, 53, was shot several times in the Todt Hill area of Staten Island on the night of March 13 before he was rushed to a hospital, where he died. Police are now investigating the matter and have yet to arrest anyone in connection.
According to NBC New York, federal prosecutors in Brooklyn had described him as the underboss of the Gambino crime syndicate and was related through marriage to the Inzerillo family in Sicily.
Police sources told The New York Times that year it was likely he died in retaliation for Castellano's killing or was the victim of a power struggle within the Gambino family. He died in prison in 2002. The New York Post reported that Cali had increased the Gambino family's involvement in drug trafficking, particularly in opioids.
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Police are looking into whether this was the work of an organized crime gang, or a faction inside the Gambino family, including John Gotti's brother, Gene, who was just released just months ago after serving 29 years for dealing heroin.
NY media say it is the first targeted killing of a mob boss in the city since 1985.
The reputed boss of the US Gambino crime family was shot to death in front of his NY home by a gunman who may have staged a auto accident to lure him outside, dying a virtual unknown compared with his swaggering 1980s-era predecessor, John Gotti. The cases resulted in long prison terms for their bosses - Gotti included - and encouraged their successors to keep a lower profile.
The New York Daily News reported in 2008 that Cali was among 62 people arrested on federal racketeering charges and he later pleaded guilty to conspiring to extort money.
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Castellano's 1985 murder was orchestrated by late John Gotti, who then became the head of the Gambino family.
Cali is the first reputed crime family boss to be shot since the execution of former Gambino head Paul Castellano in 1985.
The Genovese, Gambino, Lucchese, Colombo and Bonanno mafia families are believed to have controlled organised crime in NY for decades.
Last October, 71-year-old Sylvester Zottola, a reputed associate of the Bonanno organisation, was shot dead at a takeaway restaurant in the Bronx, New York.
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Cali spent time in prison from 2008 to 2009 on extortion charges related to a planned NASCAR race track on Staten Island.