The Stampeders confirmed Harris's death Thursday.
Harris played his entire CFL career with Calgary from 1961-72. The Hampton, Ark., native was the MVP in Calgary's 1971 Grey Cup victory over Toronto.
A West Division All-Star 11 straight seasons and an all-CFL selection eight times, he was elected to the Canadian Football Hall of Fame in 1976 and the team retired his No. 55 jersey.
In 2012, Harris was chosen to represent Calgary on a stamp that was part of Canada Post's 100th Grey Cup anniversary series.
"Wayne Harris was a great player who meant so much to this franchise and to this city," Stampeders President Gordon Norrie said in a statement. "He was also a great man who will be missed."
Harris remained in Calgary after his CFL career and worked in the oil business until 2008. His son, Wayne Jr., also played for the Stampeders and is the head coach at the University of Calgary.