The Stampeders confirmed Harris's death Thursday.
Harris played his entire CFL career with Calgary from 1961-72. The Hampton, Arkansas, native was the MVP in Calgary's 1971 Grey Cup victory over Toronto.
The CFL's top lineman a record four times an all-league selection eight times, Harris was elected to the Canadian Football Hall of Fame in 1976. His No. 55 jersey was retired in 1973, and he was voted ninth among the CFL's Top 50 players in a TSN poll in 2006.
"I would say to anybody that I think Wayne Harris was my best competitor game in and game out," former Saskatchewan Roughriders running back George Reed said. "Sometimes he had the edge and sometimes I had the edge, but there were no hard feelings. We had some really raw battles."
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."
As a senior in 1960 at Arkansas, Harris was selected the outstanding player in the Southwest Conference and played in the Cotton Bowl Classic and the All-American Bowl.
He was inducted into the College Football Hall of Fame in 2004, also is in the Arkansas Sports Hall of Fame and was named to Arkansas' all-century team.
Harris was drafted by the Boston Patriots of the American Football League, but opted to play for Calgary because Alberta better suited his lifestyle.
"Basically the decision was made because I didn't want to go East, there are too many people down there," Harris he said. "I wanted to stay in the West and I talked to a couple of guys at college who were playing up here and they really loved the CFL and told me it was really a first-class league. I'm sort of a loner and don't like a lot of people being around."
Harris said the ability to hold down a job outside of football in Canada also was a factor.
"Up here at the time you could also work, too, on top of playing football," Harris said. "You could only work out with your team once a day after training camp ended. Therefore, you could have another job on top of playing football."
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.