The 33-year-old spent five years with the New York Giants, before signing with the Bears before last season as a free agent. He signed a three-year deal with Chicago, but collected all $4.9 million in guaranteed money during his one year with the team.
With the move, the Bears clear up $2,718,750 in salary cap space.
Many NFL experts expected this move with the Bears' draft picks on day 3. The team selected safeties Deon Bush and DeAndre Houston-Carson on Saturday. Bush worked out with Rolle in the off-season, which led to the team's connection with the player.
Rolle said in a statement following his release "New York is where my heart is." He would also go on to say that if he can get back to full health, he would love to reunite with the Giants in 2016.