The release of McCourty comes one day after the Browns reached agreement on a reported four-year deal with free-agent cornerback T.J. Carrie.
Cleveland also placed wide receiver Sammie Coates on waivers, part of a roster purge by one of the busiest teams during the NFL's free agency period.
McCourty started all 14 games in which he appeared last season -- his first in Cleveland and ninth overall in the NFL. The twin brother of New England Patriots safety Devin McCourty, Jason McCourty registered 65 tackles to go along with three interceptions and two forced fumbles last season.
"Cleveland it's been real! I wish nothing but the best to the guys in that locker room!" McCourty posted on the Twitter account that he shares with his brother. "Thank you to the Haslam's and the organization for giving me the opportunity to lead and do what I love last season!"
The 30-year-old McCourty, a sixth-round draft choice of Tennessee in 2009, spent his first eight seasons with the Titans, starting 63 of 64 games during a four-year span from 2011-2014.
Carrie, who started 15 games for the Oakland Raiders last season, is expected to take over as the starting cornerback for the Browns, according to Cleveland.com.
Coates appeared in 12 games with Cleveland last season and managed only six receptions for 70 yards in 12 games. He had 21 receptions and two touchdowns for the Pittsburgh Steelers in 2016.
Also waived by the Browns were defensive lineman Ricky Ali'ifua, offensive lineman Zach Banner, defensive lineman Collin Bevins, linebacker Jeremy Cash, offensive lineman Joseph Cheek, defensive back Trevon Hartfield and running back Josh Rounds. Defensive back B.W. Webb was released.