Harrison played for Calgary from 1964 to '72 in a career that included three Grey Cup appearances and a championship in '71.
"The entire organization mourns the death of Herm Harrison," said Stampeders president Gordon Norrie in a statement. "He was a great player on the field for the red and white and an even better person off it. He will be sorely missed and we extend our condolences to his family and friends."
Harrison, a three-time CFL all-star and six-time West Division all-star, was inducted into the Canadian Football Hall of Fame in 1993.
The Arizona State University product started his pro career as a linebacker but transitioned to receiver during his rookie season.
Harrison, nicknamed "Ham Hands," had three 1,000-yard seasons and finished his nine-year career with 443 receptions for 6,703 yards and 43 touchdowns.
He still holds the team record of four touchdowns receptions, which he set in a game against Winnipeg in 1970.