Doolittle is a surname of English origin. Notable people with the surname include:
Amos Doolittle (1754–1832), American engraver and silversmith
Benjamin Doolittle (1825–1895), New York politician
Bev Doolittle (born 1947), American painter
Bill Doolittle (1923–2014), American football player and coach Colt Doolittle
Charles Doolittle (1832–1903), American Civil War general
Dorothy Doolittle (born 1946), American marathon runner
Ducky DooLittle (born 1970), American sex educator and performer
Dudley Doolittle (1881–1957), American congressman from Kansas
Eliakim Doolittle (1772–1850), American composer
Eliza Doolittle (singer) (born 1988), British singer
Emily Doolittle (born 1972), Canadian composer
Ford Doolittle (born 1941), American biochemist
Franklin M. Doolittle (1893–1979), American radio pioneer
Henry C. Doolittle (1850–1926), American judge
Hilda Doolittle (1886–1961), American poet and novelist known by her initials, H.D.