The Hall of Famer had been an analyst for the network since 2006, but he will move on after his contract expired this year. NFL Network reportedly asked Sanders to take a pay cut after also canceling his show, 21 & Prime.
"Deion has been one of the key figures responsible for the growth of the NFL Network," NFL Vice President of Communications Alex Riethmiller said in a statement. "We thank him for his work and wish him the best in the future."
Though his next step is unknown, Sanders told The Dan Patrick Show in January he was "going to be a head coach in college football next year."
He was reportedly a candidate for the job at Florida State, his alma mater, but the school instead hired Mike Norvell.