The former Liverpool boss is widely expected to replace Carlo Ancelotti at Real Madrid, after the Italian was dismissed on Monday.
Ancelotti's agent Ernesto Bronzetti claimed it is "99 percent certain" that Benitez would take over at the Bernabeu and now that appointment has edged even closer.
Napoli called a press conference for Thursday, attended by Benitez and president Aurelio De Laurentiis, where it was confirmed the Spaniard would depart.
"My time in Naples has ended. I want to thank the President and all the fans," Benitez said.
"It is always sad to leave a place where people treat you well right from the beginning."
Benitez's last game in charge of the club will be against Lazio on Sunday, with Napoli closing in on a spot in next season's Champions League.
He added: "Waiting for us on Sunday is a very important game and I want to finish my two years with a victory."
President De Laurentiis claimed Benitez "needed to live together with his family", adding further fuel to the speculation he will take over at Madrid.
The Spaniard wants to make Raheem Sterling one of his first transfer targets for Los Blancos.
Real are already one of the clubs closely watching Sterling's contract stand-off at Liverpool and will make a move given any encouragement.
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