Moe began his coaching career with the Carolina Cougars in the ABA as an assistant coach to his UNC teammate Larry Brown from 1972 to 1974. He then followed Brown to Denver, where they coached the Nuggets from 1974 to 1976. During those two seasons, the Nuggets were 125–43 (.744). They advanced to the ABA Finals in 1976, but lost to the New York Nets in six games.
After the ABA–NBA merger in 1976, Moe served as a head coach for the San Antonio Spurs for four seasons (1976–80), leading them to a conference finals appearance in 1979. He returned to Denver in 1980 to take over the head coaching reins from another UNC alum, Donnie Walsh. From 1980 to 1990, Moe compiled a 432–357 (.548) record and led the Nuggets to the postseason nine-straight years—advancing as far as the Western Conference Finals in 1985. He guided the Nuggets to two Midwest Division titles (1984–85 and ’87–88) and a franchise-record 54 wins in 1987–88. He was named NBA Coach of the Year that same year. Under Moe's direction, the Nuggets high-octane offense led the league in scoring in six of his 10 seasons in Denver. He is honored by the Nuggets with a banner that reads "432" for his number of wins as a Nuggets' head coach.