The first organist appointed to oversee the music at St Luke's was John Goss (1800-80, pictured) pupil of Thomas Attwood and a prolific composer of sacred music, including the hymn "Praise my soul, the King of Heaven" and of numerous anthems. Goss was paid the apparently generous salary of £100. His choir was made up of somewhat unruly children from a nearby church school, who sang from the West Gallery. Goss later succeeded Attwood at St Paul's Cathedral and was knighted by Queen Victoria.

Goss was replaced by an important musician of the day, Henry Forbes, who came from Chelsea Old Church. His demise twenty years later was due to his erratic organ playing, apparently attributable to the effects of alcohol!

In the latter part of the 19th century, under the influence of the Oxford Movement, the then rector of St Luke's, Gerald Blunt, announced the introduction of a paid surpliced choir stationed in the chancel. This choir played an important role in a golden period of St Luke's' history. Services with orchestra were not uncommon, and Sunday evening concerts brought many thousands to the church. The director of music of the time was Everard Hulton, a recommendee of John Stainer, who was in post for 34 years.

In 1904, St Luke's appointed another famous organist as Director of Music: John Ireland (1879-1962, pictured). He was a prolific composer, and his works include chamber music and piano sonatas as well as organ and choral music, such as the anthem "Greater Love Hath No Man" and the hymn "My Song is Love Unknown". Under Ireland, Evensong was sung daily by boys from the church school.

Ireland -- who, as evidenced by some of his correspondence, was never really happy at St Luke's -- departed in 1926, and was succeeded by Guy Eldridge. Until the onset of World War II the music tradition continued to thrive, with a choir made up of twelve men and about sixteen boys, but lack of financial support meant that the choir gradually dwindled after this. Eldridge's call up to the RAF in 1941 left two students to run the wartime music, one of whom was Michael Howard, later of Ely Cathedral. He was replaced in 1945 by Geoffrey Bush, who found it next to impossible to recruit choirboys.

Despite an attempt at revival in 1954 under the direction of Leslie Wigg and subsequently of Peter Chapman (1967-1985), the number of boys singing dropped drastically, and in 1985 the decision was taken to replace them with women, enabling John Halsey to lay solid foundations for a restored tradition. He was succeeded by Jeremy Filsell, a former Oxford organ scholar and Assistant Organist at Ely Cathedral, under whose direction the first choir recording, "Music from St Luke's Chelsea", was made in 1993. Following his untimely departure in 1994 he was succeeded by Nicholas Ansdell-Evans. When he in turn left three years later to devote more time to his composing, St Luke's acquired its first female, and first American, Director of Music, Anne Elise Smoot, previously Assistant Organist at St Giles's, Cripplegate. Among the accomplishments of her tenure was the choir's second recording, "O be joyful in the Lord", in 1999. Unfortunately her increasingly successful career as an organist, with attendant recital and recording commitments overseas, became impossible to combine with her duties. She was succeeded briefly by Ben Nicholas (now at Tewkesbury Abbey), then in December 2000 by Jonathan Leonard and in 2011 by Jeremy Summerly.