No description of a suspect is now available, and no arrests have been made, according to an NYPD spokesman.
NY media reported that 53-year-old Cali was shot multiple times outside his auto on Staten Island on Wednesday evening, local time, by an unidentified man who then fled the scene in a blue vehicle.
Cali was rushed to Staten Island University North Hospital, where he was pronounced dead.
In January 1997, an Federal Bureau of Investigation agent reportedly notified Italian police of Cali's distinctive standing as a member of crime families on both sides of the ocean, after he was "combined" into the Gambino family.
Infamous mob boss Francesco "Franky Boy" Cali has died.
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.
Cali was said to have strong ties to the Sicilian Mafia, and experts suggested that his ascension was part of an attempt by the Gambinos to lower their high-profile image created by former godfather John Gotti. That hit was ordered by Gotti, who later took over the family until being convicted of racketeering and Castellano's murder in 1992.
Cali, who served on the family's ruling panel for several years, was elevated to acting boss in 2015, replacing then 68-year-old Domenico Cefalu.
He had just one criminal conviction: an extortion charge in 2008 for an attempted shake down of a trucker working at a proposed NASCAR race track in Staten Island.
It was a marked change from the Gotti era, which brought with its unnecessary attention and exposure. The house is listed under the name of Rosaria Inzerillo.
NY media say it is the first targeted killing of a mob boss in the city since 1985.
He rose quickly through the ranks of organized crime, becoming a powerful capo before the age of 40, less than a decade after he became an inducted member, according to court papers.
The last mob boss to be killed was Paul Castellano, also the leader of the Gambino crime family at the time, who was murdered outside Sparks Steakhouse in Midtown Manhattan in 1985.
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