On Wednesday, a little after 9 p.m., Cali - who went by Frank rather than Francesco- was shot multiple times in the torso outside of his Staten Island home, New York Police Department confirms to PEOPLE. He was rushed to a local hospital, where he was pronounced dead.
A witness told The New York Daily News: 'There were like six shots, and then there were three more.
The circumstances preceding the shooting weren't immediately known, but police say they're looking for a blue pickup truck that fled the scene.
Cali was the first NY crime family boss shot since 1985, when Paul Castellano, who owned a mansion on Todt Hill, was executed as he arrived at Sparks Steakhouse in Manhattan, according to Pix 11.
'The man was on the ground face-up.
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In 2008, Cali was arrested and charged with federal racketeering as part of Operation Old Bridge - a code name for the February 7 arrests in Italy and the US that targeted the Gambino crime family.
NY media say it is the first killing of a family boss in the city since the Gambino family's Paul Castellano was shot dead outside a restaurant in 1985 on the orders of John Gotti.
The Gambino crime family is one of what is widely referred to as "The Five Families" of Italian organized crime operations in New York City and other parts of the United States.
It is believed he only had one criminal conviction, for conspiring to extort money in 2008 for which he served 16 months in prison.
The Genovese, Gambino, Lucchese, Colombo and Bonanno mafia families are believed to have controlled organised crime in NY for decades.
Castellano was killed on Gotti's orders, in what was seen to be a major break from Mafia protocol, which forbade the unsanctioned murder of a family head. John Gotti and his turncoat underboss, Sammy "Bull" Gravano watched the action from Third Avenue.