He held several posts at the University of Manchester and at the Royal Manchester College of Music, delivering the first lecture on the opening of the latter institution in 1893. He became the first Professor in the Art and Practice of Teaching at the RNCM, resigning in 1918 to become Manchester's first Music Adviser.
It is his music for children, however, written originally for his daughters Elsa and Ida, which is Carroll's claim to enduring fame. After Scenes at a Farm, published by Forsyth Brothers Ltd in 1912, came all the other sets over a period of forty one years. These included The Countryside (1912), Sea Idylls (1914), Forest Fantasies (1916), Water Sprites (1923), and River and Rainbow (1933). The uniqueness of Carroll's brilliant idea was to fire the child's imagination by uniting what he called the Sister Arts: by simultaneously stimulating the child visually and poetically as well as musically.