Defensive tackle Stephen Paea also informed the team that he is retiring from football, ESPN's Adam Schefter reported. Paea signed a one-year contract with the Cowboys in March.
Carroll, a defensive back, signed a three-year, $10 million deal that included a $3 million signing bonus after starting 16 games last season for the Philadelphia Eagles.
The 30-year-old Carroll has not suited up for the Cowboys since sustaining a concussion in a 42-17 loss to the Denver Broncos in Week 2. He has made five tackles this season.
Carroll, who may also be facing a suspension after being arrested for DUI this offseason, is free to sign with any team.
Jourdan Lewis, a third-round pick of the 2017 draft, has fared well with the Cowboys (2-3), who also feature Orlando Scandrick and Anthony Brown as the starting cornerbacks. Second-round selection Chidobe Awuzie was shuffled to safety during Sunday's 35-31 loss to the Green Bay Packers.
Paea, 29, collected four tackles in the first four games of the season before sitting out Sunday's clash versus the Packers with a knee injury. He has 129 tackles and 14 sacks in 83 career games with the Cleveland Browns, Washington Redskins, Bears and Cowboys since being selected by Chicago with a second-round pick in the 2011 draft.