The veteran wide receiver tweeted Thursday night: "its official, I personally wanna thank all the fans who stuck with me in jacksonville for the last 4 years but sorry to say my time is up!!"
Sims-Walker finished third on the Jaguars with 562 receiving yards and second with seven touchdowns last season.
Pro Bowl tight end Marcedes Lewis signed a one-year franchise tender Thursday night.
Lewis will earn $7.3 million in 2011, although the team still could sign him to a long-term deal after a new collective bargaining agreement is in place.
Lewis had 58 receptions for 700 yards and 10 touchdowns last season. A first-round draft pick in 2006, Lewis has 181 career catches for 2,224 yards and 17 touchdowns.
Information from The Associated Press was used in this report.