Cali's body was found in an area of Staten Island that has been home to some of New York's most notorious mobsters and their families.
Cali, 53, was fatally shot outside his Staten Island home Wednesday night.
"There are multiple, multiple angles that we are exploring", Shea said at a news conference at police headquarters. "Were others conspiring to do this crime?"
Surveillance video of the killing showed a man, allegedly Comello, crash his auto into Cali's parked SUV, drawing Cali outside in what might have been a ploy to lure him out of the house, Shea said. He was shot six times before reportedly being run over.
Police said surveillance video captures the shooter, and the pick-up believed to be the getaway truck. For one, a 24-year-old man from Brick, New Jersey has already been arrested in connection with the murder.
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Investigators in NY are searching for an attacker who killed an alleged gangster, Franky Boy Cali, outside his home on Wednesday night. His brother and brother-in-law are both believed to be involved in organized crime, as well. News accounts since 2015 said he had ascended to the top spot.
His only mob-related criminal conviction came a decade ago, when Cali pleaded guilty in an extortion conspiracy involving a failed attempt to build a NASCAR track on Staten Island. He was sentenced to 16 months behind bars and was released in 2009.
Police fear the murder of Cali will provoke revenge attacks.
The shooting is reminiscent of the 1985 murder of another Gambino crime boss, Paul Castellano, who was gunned down outside a popular New York City steakhouse in 1985.
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