The anchor will host her own daytime news and discussion program at NBC, as well as presenting an in-depth Sunday night news show.
The move deprives Fox News of its second most-popular host after Bill O’Reilly.
Megyn Kelly’s contract with Fox was due to end later this year.
She was pushed into the international spotlight in 2015 when she accused Donald Trump of misogyny during a Republican presidential debate.
Megyn Kelly later said that she would “not apologize for doing good journalism”, following criticism from Donald Trump’s supporters.
NBC News chairman Andrew Lack called Megyn Kelly “an exceptional journalist” who has “demonstrated tremendous skill and poise”.
“We’re lucky to have her,” Andrew Lack said.
Further details of Megyn Kelly’s news programs will be unveiled by NBC in the coming months, the company said in a statement on January 3.
Megyn Kelly, a lawyer-turned-journalist, joined Fox News’ Washington bureau as a correspondent before being given her own prime-time show, the Kelly File.
The New York mother-of-three began her career as a local news reporter in 2003, after nine years in law.
During the election campaign, Megyn Kelly challenged Donald Trump on his statements about women.
Megyn Kelly’s accusation of misogyny against Donald Trump made her a target for his supporters and the subject of attacks from the billionaire himself.
Donald Trump accused Megyn Kelly of having “blood coming out of her wherever”, later denying he was referring to menstruation.
In a move described by Fox News as “unprecedented”, Donald Trump later refused to participate in shows hosted by Megyn Kelly.
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