Sharpe began his athletic career as a student at the William Penn Charter School in Philadelphia.

"[3] In 1929, sports writer Lawrence Perry wrote that Sharpe was best recalled for a 50-yard dropkick in the 1899 Yale-Princeton game.

In February 1898, Sharpe led Yale's basketball team to a 27–7 win over New York's Knickerbocker Athletic Club.

A newspaper account of the game praised Yale for its "signal work" in passing the ball from one to another without a hitch.

"[6]In January and February 1899, Sharpe played left forward and center on a Yale basketball team that played games against teams from the New Britain Athletic Club, the Fourth Separate Company of Yonkers, and Trinity College.

[11][12] After returning from the Western trip, Sharpe led Yale to a 30–10 victory over the Dreadnought Athletic Club—a New York team considered one of the best in basketball at the time.

... Sharpe could row, run a fine relay, jump, put the shot, and, in fact, do about anything on the athletic field.

In 1901, Sharpe accepted a position as the director of physical education at the William Penn Charter School.

He was quoted as saying that young men in the United States needed football, because it was "the only game in which a gentleman can fight.

In February 1912, Sharpe was hired by Cornell University where he served as the coach of the football, basketball and baseball teams.

Menke wrote:"Al Sharpe at Cornell started the season with only one real star from his 1914 eleven -- Charles Barrett, the amazing quarterback.

Sharpe has made a reputation since he became the dominant figure in Cornell athletics as the greatest all round coach in the country.

[25] In March 1921, Sharpe announced that he would resign as Yale's athletic director when his contract expired in June.

[17] While at the Ithaca school, Sharpe also developed a reputation as one of the leading football and basketball officials in the East.

[1] When he was hired at Washington University, sports writer Lawrence Perry wrote: "No athletic director and coach coulc by any possibility have more friends pulling for him than this former Yale backfield star whose character is so outstanding that no young men ever came in contact with him without being better for it.

[29] In the 1930s, Sharpe was also the president of the Touchdown Club, an organization of former football players, and an executive with the Red Cross.