Carroll taught himself how to play the piano and began playing in movie houses before he finished grade school. After he graduated from high school, he moved to New York City, where he worked as an arranger in Tin Pan Alley and at night entertained at the Garden Café and accompanied various vaudeville shows.
In 1912, Carroll was hired by the Schubert brothers' Winter Garden productions as a contract writer. He worked with Arthur Fields to produce his first hit, On the Mississippi. He wrote several Broadway stage scores including some popular favorites: "I'm Always Chasing Rainbows" (based on a section of Fantaisie-Impromptu by Frédéric Chopin), "By the Beautiful Sea" and "The Trail of the Lonesome Pine". Harry married Anna Wheaton and together they had one child. Later he moved west to Los Angeles and became involved in early movies. He served as the director of ASCAP from 1914 to 1917.
He died on December 26, 1962, in Mount Carmel, Pennsylvania.
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