Thursday's move had been expected because the Cardinals wanted to avoid paying him the $4 million roster bonus and $8 million salary he is due.
General manager Rod Graves has indicated the team would be interested in re-signing Rolle. Inside linebacker Karlos Dansby, who became an unrestricted free agent after being given the franchise tag the past two years, may also leave.
In addition, Arizona tendered one-year qualifying contract offers to five players -- wide receiver Steve Breaston, guard Deuce Lutui, center Lyle Sendlein, tight end Ben Patrick and nose tackle Gabe Watson.
Rolle was Arizona's first-round pick, the eighth selection overall, out of Miami in 2005. He began his pro career as a cornerback but had most of his success after being switched to safety in 2008.
In 68 regular-season games, 59 as a starter, Rolle had 12 interceptions, four forced fumbles and 1½ sacks. In six postseason games, Rolle had an interception and a fumble recovery.
Breaston received a first-round tender, which means that if another team makes an offer that Arizona decides not to match, the Cardinals would get a first-round draft pick as compensation. The other four players got second-round tenders, which gives Arizona the option of matching any offer or receiving a second-round draft pick from that team as compensation.
The two-time NFC West champions had a number of personnel issues to resolve as free agency approached. Starting left tackle Mike Gandy is a free agent and Matt Leinart is the lone quarterback under contract.
The Cardinals historically have not gone for a big name in free agency, opting instead to spread their money around.