Originally a member of several rock groups around Liverpool, such as The Assassins and The Profiles, Molland began his recording career in 1965 when he joined The Masterminds. This group released a single on Immediate Records IM 005, consisting of a cover version of Bob Dylan's "She Belongs to Me" backed with a band original, "Taken My Love". After this the group disbanded and Molland joined the backing group of The Merseys. Although never recording with them, he did accompany them on tour.