His murder is the first of a NY mob boss since Paul Castellano was famously assassinated at Sparks Steakhouse in 1985.
The 53-year-old, thought to have been de facto godfather of the Italian crime family since 2015, suffered "multiple gunshot wounds to the torso" in the attack on Wednesday evening, police said.
He was pronounced dead at a hospital.
Police said surveillance video captures the shooter, and the pick-up believed to be the getaway truck.
In 1992, Gotti was convicted in Castellano's murder and a multitude of other crimes.
Now, authorities are turning a watchful eye to just-out-of-jail Gene Gotti, brother of the late John Gotti, who was released from prison six months ago after serving 29 years for dealing heroin, reports the New York Daily News.
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According to local media in NY, he took the helm of the Gambino family in 2015, replacing Domenico Cefalu.
"Anybody who was making a move on boss of a crime family - besides a one-off renegade, you know, insane character - would have to have the backing of captains in that crime family".
Cali was the first NY crime family boss shot in 34 years, according to WPIX.
Shea said there has been a slight uptick in alleged mob-related violence in NY within the previous year.
Cali shunned the limelight even after becoming don, ruling from the top while lying low in his affluent Todt Hill neighborhood in Staten Island, where Castellano also held court.
It wasn't the first such spattering of gore in recent years, however.
He then allegedly returned to the scene of the crime hours later to grieve with the older man's family.