Harris, who turns 31 in June, was one of the longest-tenured Broncos, having made the roster as an undrafted rookie in 2011 -- the same year John Elway started his tenure as the team's top football decision-maker.
Harris is a four-time Pro Bowl selection and is the final member of the "No Fly Zone'' secondary that was part of the Broncos' Super Bowl 50 win to move on from the club.
The relationship between Harris and the Broncos fractured a bit last spring when he stayed away from the start of the team's offseason workouts in a contract dispute. Harris had been seeking a new long-term deal, but eventually signed a reworked, one-year deal for $12.05 million for the 2019 season.
Injuries in the Broncos' secondary forced the Broncos to play Harris outside much of the time instead of in the slot where he has said he's "still the best in the league in there."
He said he had increasingly grown weary of the Broncos' struggles on the field as the team has had three consecutive losing seasons for the first time since the 1970s and has missed the playoffs sur consecutive years.
Harris has played at least 15 games in eight of his nine seasons for the Broncos and Denver was ranked among the league's top five in pass defense in 2015, 2016 and 2017. In 2015 the Broncos defense led the league in almost every major category, including pass defense. He has 20 interceptions, 86 passes defensed, 6 forced fumbles and 4.5 sacks in his career.
ESPN's Jeff Legwold contributed to this report.