Rolle, 33, broke into the NFL with the Tennessee Titans in 1998 and went to the Pro Bowl in 2000. He joined the Ravens in March 2005 and started all 16 games during his first two seasons in Baltimore.
But things began to go awry in 2007, when Rolle was diagnosed with epilepsy. That, and a shoulder injury, limited him to six games that season.
He missed six starts in 2008 because of neck problems and had surgery during the offseason. He was released before the 2009 season at his own request, then re-signed a four-year, $10 million contract.
Last August, however, Rolle was placed on the physically unable to perform list, where he remained for the entire season.
Ravens general manger Ozzie Newsome told Rolle about a week ago that he planned to terminate his contract.
"I'm glad to have the opportunity to know Samari," Newsome said Tuesday. "We know the incidents and what happened toward the end of his career that maybe shortened it. I don't know where he's at with that."
It is likely Rolle will retire, given the serious nature of his neck injury.
"I had a chance to get to know him through some of those end-of-career issues that he had here mostly last year and the beginning of this year," coach John Harbaugh said. "The way he carried himself, the way he handled adversity, the way he fought through the medical issues, the injuries ... Just a true class individual."
Rolle has played in 148 games. He has 31 career interceptions, one touchdown and 9½ sacks.