Other notable cuts were linebacker Ryan Nece and receiver Michael Spurlock, who last season became the first player to return a kickoff for a touchdown in the Bucs' 31-year history.
The 28-year-old Simms has not played in a regular-season game in nearly two years and entered training camp fourth on the depth chart behind Jeff Garcia, Brian Griese and Luke McCown. Saturday's move left rookie Josh Johnson as the fourth quarterback.
Simms missed the final 13 games of 2005 after taking several hard hits and having his spleen removed hours after a loss to the Carolina Panthers. He spent much of last season on injured reserve when he was slow to regain his pre-injury form.
The sixth-year pro, who took over for an injured Griese and helped the Bucs win the NFC South in 2005, asked to be released during the offeason, saying a soured relationship with coach Jon Gruden was beyond repair.
He appeared in three preseason games, completing 19 of 30 passes for 155 yards, no touchdowns and one interception.
The Bucs also released receivers Brian Clark and Chad Lucas; running backs Kenneth Darby and Clifton Smith; fullback Carl Stewart; guards Phil bogle, Chris Denman and Brian Johnson; tackles Dennis Roland and Chris Clark; cornerbacks Marcus Hamilton and Darrell Hunter; defensive tackles Dre Moore and Chris Bradwell; defensive ends Charles Bennett and Patrick Chukwurah, and tight end Daniel Fells.