Donohue was the head coach of the senior Canadian men's national basketball team for 16 years, and he led them to several international successes.

Donohue served as a basketball coach for St. Nicholas of Tolentine High School.

At Power Memorial, Donohue had a career win–loss record of 163–30, including winning 71 straight games with the star center of his team, Lew Alcindor (later known as Kareem Abdul-Jabbar).

Donohue coached Canada at three Summer Olympic Games (in 1976, 1984, and 1988), highlighted by two fourth-place finishes in 1976 and 1984.

In an incident aimed at motivating gameplay, Donahue made a racially inappropriate remark directed at Kareem Abdul-Jabbar by calling him a "n*gger", resulting in a strained relationship between the two.