Agent Hadley Engelhard said Williams died Tuesday morning at St. Joseph's Hospital in Tampa, Florida.
Williams had been hospitalized in intensive care after an accident at a construction site in Hillsborough County, which includes Tampa, that left him partially paralyzed. The Tampa Bay Times, citing Tierney Lyle, the mother of Williams' 8-year-old daughter, reported he was taken off a ventilator Thursday.
Williams was from Buffalo, New York, and played nearby at Syracuse University.
He burst onto the scene in 2010 as a fourth-round pick with the Tampa Bay Buccaneers, catching 65 passes for 964 yards and 11 touchdowns. His touchdown-reception total set the single-season club mark at the time for any player, and he wound up second in Offensive Rookie of the Year voting.
"We are saddened to hear of the untimely death of Mike Williams, which has left our organization, his former teammates and fans with heavy hearts," the Buccaneers said in a statement. "We send our deepest sympathies to his family and loved ones as they mourn this tragedy."
Williams finished his career with 223 catches for 3,089 yards and 26 touchdowns in 63 games (52 starts) across four years with the Buccaneers and one with the Buffalo Bills (2014).
Williams was last on an NFL roster during a portion of the 2016 offseason with the Kansas City Chiefs.
The Associated Press and Reuters contributed to this report.
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