Collins, 29, signed a four-year, $50 million contract with the team in 2017 after being traded from the New England Patriots in 2016. The second round pick in the 2013 NFL Draft had 104 tackles, four sacks, four passes defensed, a forced fumble, fumble recovery and an interception in 16 starts last season for Cleveland.
The veteran defender was set to make $10 million in 2019 and had a $500,000 bonus headed his way. The Browns saved $9.25 million in salary cap space by making the move.
"We want to thank Jamie for his contributions to the Cleveland Browns," Browns general manager John Dorsey said in a news release.
"These types of decisions are never easy. Jamie is a respected veteran player in this league and we wish him the best as he continues his career."
The 6-foot-3, 250-pound linebacker made his lone Pro Bowl in 2015, after making 89 tackles and tallying six passes defensed. He also had five sacks, a league-high five forced fumbles, a fumble recovery and a touchdown in 12 starts that season for the Patriots.
Collins kept it simple in his farewell to Cleveland, tweeting: "Thanks for everything, Browns."
Collins won a Super Bowl with the Patriots in 2015.