Sylvia May Moore was born into a clergyman's family in Wimbledon, South London in 1880. She qualified from the London School of Medicine for Women (now the Royal Free Hospital) in 1906. In 1908 she married Jack Payne, a surgeon, with whom she had three sons. During the First World War she was Commandant and Medical Officer in charge of Torquay Red Cross Hospital which received wounded soldiers direct from the battle lines. She was awarded a CBE in 1918 for her services.

During the war she also became interested in psychoanalysis and began training with James Glover at the Brunswick Square Clinic in London. She later also underwent a short period of analysis with Hanns Sachs in Berlin, where she came to know Karl Abraham. Payne became an Associate Member of the British Psychoanalytical Society in 1922 and a Member in 1924. She played an increasingly important role in the practice, advocacy and administration of psychoanalysis. She played a key role in the Controversial Discussions, becoming President of the Society from 1944 to 1947 and again from 1954 to 1956. She was also a fellow of the British Psychological Society and chairman of its Medical Section. She was elected an honorary member of the BPAS in 1962. She died in 1976.