Marrone will take over as Bills head coach less than a week after the firing of predecessor Chan Gailey, who compiled a 16-32 record over three seasons.
The 48-year-old former Syracuse mentor guided the Orange to a 25-25 record in four seasons, helping to turn around a team that was 10-37 prior to his arrival.
He finished his stint with Syracuse with a 38-14 victory over West Virginia in last month's Pinstripe Bowl at Yankee Stadium in New York.
Marrone has also served as offensive line coach for the New York Jets and as offensive coordinator for the New Orleans Saints from 2006-08.
The Bills also interviewed Oregon Coach Chip Kelly, former Chicago Bears Coach Lovie Smith, former Cardinals Coach Ken Whisenhunt and current Cardinals defensive coordinator Ray Horton, the News said.