The New York Post reported that police sources said the shooter hit Cali with multiple bullets and a 911 caller said they heard six or seven shots.
He described the suspect as an adult male who sped off in a pickup truck.
Police added he was taken to Staten Island University North hospital, where he was pronounced dead.
"He has a conversation with an individual in front of that residence and that individual at some point in time, it's only about a minute into it, pulls out a firearm and shots are fired", said NYPD Chief of Detectives Dermot Shea.
The last crime family boss to be shot in NY was Paul Castellano, who was also a Gambino crime boss.
Suspected Gambino crime boss Frank Cali was fatally shot outside his home in NY on Wednesday.
Rising Gambino family mobster John Gotti allegedly ordered the hit on Castellano.
Francesco Cali, the reputed boss of the Gambino crime family, was fatally shot outside his Staten Island home Wednesday night, a senior police official said. After Gotti went to prison, Cali eventually took over the organization.
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Aggressive federal prosecutions in the past 25 years have decimated the ranks of New York's five Mafia families.
The post-Gotti chapter saw the mob's influence on the U.S. eastern seaboard wane - but Wednesday's hit threw NY back to its golden years of organized crime.
Cali was an associate in the Gambino family, according to court documents, when he was indicted in 2008 with more than two dozen other Gambino members for a range of alleged crimes. He served a 16-month sentence.
"We thought those days were over", Mayor Bill de Blasio said of Cali's slaying.
New York's major crime families, the Gambinos, the Luccheses, the Genoveses, the Bonannos and the Colombos, have seen some decline over the past few decades, as federal law enforcement agencies have tried to extricate their influence from construction and other major industries. "But I guess old habits die hard".
Last October, 71-year-old Sylvester Zottola of the Bonanno family was shot dead while waiting in his vehicle for an order from a Bronx McDonald's.
A week ago, Persico died after serving 33 years in prison.