LeGrand, 21, was injured while playing for Rutgers in a game against Army on Oct. 16, 2010. The injury was diagnosed as fractures of two cervical vertebrae.
While he was determined to be paralyzed from the neck down, he has since regained some movement. LeGrand, however, still uses a wheelchair.
He was signed by Tampa Bay, now coached by former Rutgers Coach Greg Schiano, May 2.
"This small gesture is the least we could do to recognize his character, spirit and perseverance," Schiano said at the time. "The way Eric lives his life epitomizes what we are looking for in Buccaneer Men."
The Buccaneers announced LeGrand's retirement Thursday.
"Making it to the NFL was my dream. But now I want to see my team as strong as possible at the start of training camp," LeGrand said in a release. "I'm a Buc for life."
LeGrand was given the Jimmy V Perseverance Award at the ESPYs July 11 and last month was presented the Unsung Hero Award by the New Jersey Hall of Fame.