The club released the colorful Valverde from his contract with Triple-A Toledo on Wednesday, ending a stay that included several highs and lows.
"We tried and he tried and it just didn't work," Tigers manager Jim Leyland said. "I'll always have great memories of him. He did a terrific job for this organization. He was a terrific closer and a terrific teammate."
The peak of Valverde's time in Detroit came in 2011 when he was 49 for 49 in save chances. He saved 35 games last season, but faltered in the playoffs and became a free agent.
He didn't sign with another team and Detroit eventually brought him back on a minor league deal, calling him up to the majors in late April.
Valverde went 0-1 with a 5.59 ERA, converting nine saves in 12 chances, but it never seemed easy and he was designated for assignment on June 21. He accepted a trip to Toledo, where he had seven saves with a 4.09 ERA in 11 games.
Leyland will always remember Valverde's performance in 2011.
"That's one of those freak years that comes around every now and then, not too often obviously," Leyland said. "That's pretty impressive."
Valverde had a nightmarish postseason in 2012. He got a save in the division series against Oakland, but allowed three runs in 1 2-3 innings in two appearances.
Valverde gave up three runs in two-thirds of an inning in his only appearance in the ALCS against New York, forcing Leyland to remove him from the closer's role. Valverde pitched just once in the World Series against San Francisco, allowing two runs in one-third of an inning.
Joaquin Benoit has taken over as Detroit's closer and was 13 for 13 in save opportunities going into Wednesday's game.