With the North Carolina Tar Heels, Dooley won three Atlantic Coast Conference titles, including the school's first outright conference championship in 1971. He left North Carolina as the winningest coach in school history, though he has since been passed by Dick Crum. He is still tied for second on the school's wins list, behind Mack Brown, and is still the school's longest-tenured head coach. He also achieved the school's first 11–win season in 1972. Only two other Tar Heel teams have ever won 11 games.
After his tenure at North Carolina, Dooley served as the athletic director and head football coach at Virginia Tech. He led the Hokies to three bowl games--as many as they had attended in their entire history prior to his arrival. His best team was the 1986 unit, which went 10-1-1 and won the Peach Bowl.
His tenure at Virginia Tech, however, ended shortly afterward amidst allegations of NCAA recruiting violations. After resigning from his positions at Virginia Tech, he sued the university for $3,500,000 alleging breach of contract. The lawsuit was settled out of court. At the time, he was the winningest coach in school history, though he has since been surpassed by his successor, current coach Frank Beamer.
Finally, Dooley served as the head coach at Wake Forest where, as of January 2010, he is third in the football program's history for all-time wins and tied for fourth in longest tenure.