[2] Moe was selected in the NBA draft in 1960, by the Detroit Pistons, and again in 1961, this time by the Chicago Packers, but began his professional career in Italy's Lega Basket Serie A with the Pallacanestro Petrarca Padova.

He garnered ABA All-Star honors three times in an injury-shortened five-year professional playing career.

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.

Moe 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.

Under Moe's direction, the Nuggets high-octane offense led the league in scoring in six of his 10 seasons in Denver.

Moe announced his dismissal from the Nuggets on September 6, 1990, at a press conference where he and his wife Jane had a Champagne toast.

He had three years remaining on his contract but was caught in the middle of a front-office restructure initiated by Comsat Video Enterprises, Inc. which had purchased the franchise eleven months earlier.

"[6] Moe's passing strategy was adopted from North Carolina head coach Dean Smith.

[6] Though his offensive strategy led to high scores, Moe's Denver teams were never adept at running fast breaks.

He disputed the fact that his teams did not play defense, attributing the high scores to the pace of the game.