Leif Mortensen was one of the most successful amateur cyclists in Denmark in the 1960s. In 1963 Mortensen finished second in the junior individual time trial at the national championships, before winning the youth team time trial title at the Nordic Championships one year later. In 1967 he won his first medal at the UCI World Championships with silver in the amateur team time trial. His performances earned him a place on the Olympic team for the Mexico City Games, where he finished second in the road race and fourth in the team time trial. Mortensen then had double success at the 1969 World Championships, winning gold in the amateur road race and silver in the team time trial.
Mortensen then turned professional, winning silver in the road race at the 1970 World Championships in Leicester, England, finishing only two seconds behind Jean-Pierre Monseré. Throughout the first half of the 1970s he had multiple podium and top-ten finishes, including placing sixth overall in the general classification of the 1971 Tour de France. As a professional, however, his wins became more and more sporadic, with him eventually retiring in 1975. In 1994 Mortensen was inducted into the Danish Sports Hall of Fame.