The NYPD said they responded to a 911 call of an assault in the upscale neighborhood of Todt Hill, and they found the victim with multiple gunshot wounds when they arrived.
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.
Infamous mob boss Francesco "Franky Boy" Cali has died.
Cali himself was jailed for 16 months for his connection to an extortion scheme surrounding an attempt to build a NASCAR track on Staten Island.
Police sources reportedly said the shooter fled the scene in a blue pickup truck.
According to reports, Cali's death marks the highest ranking member of a NY crime family to be murdered in decades.
The New York Daily News reported in 2015 that cali had been made acting boss of the Gambino crime family: "Frank Cali, 49, of Staten Island, who has served on the family's ruling panel for several years, has been elevated to acting boss, replacing 68-year-old Domenico Cefalu, the website Ganglandnews.com reported Thursday".
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It was a marked change from the Gotti era, which brought with its unnecessary attention and exposure.
According to a 2008 Advance report, Cali - who also went by "Franky Boy", - was born in Brooklyn and married into the Inzerillo family of Palermo and cultivated close ties with members of the Siderno cartel in Italy.
Rudolph W. Giuliani, who at the time was the United States Attorney for the Southern District of NY, condemned the killings and vowed to find those responsible.
The investigation exposed a drug trafficking partnership between the Gambinos and the Sicilian Mafia.
According to the Associated Press, court documents referred to Cali as the underboss of the Gambino crime family.
Cali's wife and children were home at the time of the shooting.
On June 4, 2008, Cali pleaded guilty to conspiring to extort money.