Barrymore also composed music. His works ranged from solo piano pieces to large-scale orchestral works, such as "Tableau Russe," which was performed twice in "Dr. Kildare's Wedding Day" (1941) as Cornelia's Symphony, first on piano by Nils Asther's character and later by a full symphony orchestra. His piano compositions, "Scherzo Grotesque" and "Song Without Words", were published by G. Schirmer in 1945. Upon the death of his brother John in 1942, he composed a work "In Memoriam", which was performed by the Philadelphia Orchestra. He also composed the theme song of the radio program "Mayor of the Town".