Moss served as head baseball coach and backfield coach at the University of Miami in 1955 and University of Wisconsin–Madison in 1958. In 1959, he was named as the head football coach and athletic director at Florida State, and compiled a 4–6 record and later at Marshall University in 1968 where he compiled an 0–9–1 record before resigning in the wake of NCAA recruiting violations. From 1960 through 1962 he was head coach of the Montreal Alouettes in the Canadian Football League. In the mid-1960s and again in the early 1980s he coached the West Virginia Rockets of the semi-pro American Football Association. In 1987, Moss was hired as the head coach of the Chicago Bruisers of the Arena Football League. In 1991, he was named as first coach of the Orlando Predators of the Arena Football Leagu