Moore began his coaching career at Corsicana High School under Texas high school coach Jim Acree. In 1965, he became assistant coach at SMU. After the 1972 season, he joined the Nebraska Cornhuskers as receivers coach, becoming offensive coordinator under coach Tom Osborne in 1978. In 1979, at North Texas State, Moore got his first head coaching job. After two seasons he left North Texas for Texas Tech, where he spent five seasons and garnered a record of 16–37–2 before being replaced by David McWilliams. After three years away from football, Moore joined the coaching staff at Arkansas where he remained for two seasons before taking the head coaching position at Appalachian State in 1989. During his tenure of twenty-four years as head coach at Appalachian State, Moore led the Mountaineers to ten Southern Conference championships and three consecutive NCAA Division 1-AA national championships. The 215 ASU victories under his leadership is a school record. On September 1, 2007, Moore led Appalachian State to score one of the biggest upsets in college football history, defeating the then fifth-ranked Michigan Wolverines 34–32 at Michigan Stadium. This marked the first time a team in a lower subdivision defeated a ranked team in a higher subdivision. It was also the first game and loss for Michigan against a Division I FCS team. Moore had learned the spread offensive scheme that enabled him to defeat Michigan from then-West Virginia coach Rich Rodriguez, whom Michigan hired to succeed Lloyd Carr the following season. Moore became the 28th head coach in Division I history to reach 200 wins after the Mountaineers defeated the Furman Paladins on October 25, 2008. On December 2, 2012 after a first round home playoff loss to Illinois State, athletics director Charlie Cobb announced that Moore would not return for the 2013 season. According to a press release issued by the ASU athletic department, Cobb stated that he and Moore agreed after the end of the 2011 season that the 2012 season would be Moore's last as head coach, but chose not to make an announcement until that time. However, several days later, Moore claimed that there had been a communication gap, and that he had wanted to coach for one more season in 2013. Cobb announced that assistant head coachScott Satterfield, who played quarterback under Moore at Appalachian from 1993 to 1995 and served as an assistant at ASU from 1998 to 2008, would serve as interim head coach while a national coaching search was conducted. Satterfield was given the permanent job on December 14, 2012.