"There are no arrests and the investigation is ongoing", police said in a statement.
Most likely, he was already dead by the time the pickup sped away into the night.
Someone called 911 about the crash - in addition to other calls about shots fired out on the street, sources said.
Fox News noted, "Cali, who had roots in Sicily and ties to the Sicilian Mafia, was the highest-ranking organized crime figure to be murdered in New York City since 1985, when Paul Castellano was assassinated as he arrived as Sparks Steakhouse in Manhattan, according to WPIX-TV".
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.
Castellano's death led to the rise of John "Dapper Don" Gotti, who then took over as Gambino family boss, running criminal enterprises ranging from gambling to money laundering to prostitution.
The head of the Gambino crime family was shot and killed outside his home in Staten Island on Wednesday night, according to NY media reports.
Cali served a 16-month prison sentence for the crime. He was convicted of racketeering and murder in 1992 and later died in prison. Now, there is concern that this could be the start of a mob war in New York City.
The Gambino family is one of New York's five historic Italian Mafia families - along with the Genovese, Lucchese, Colombo and Bonanno families.
Federal prosecutors referred to Cali in court filings in recent years as the underboss of the Mafia's Gambino family, once one of the most powerful and feared crime organisations in the country.
In October, Sylvester Zottola, 71, a reputed associate of the Bonanno crime family was shot and killed as he waited in his SUV to pick up an order at the drive-through window of a McDonald's in the Bronx.
A witness said that his family members rushed outside after Cali was gunned down.
A week ago, Persico died after serving 33 years in prison.
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