Lilian Sharpley was born on March 22, 1901 to Arthur Croft and Thomas "Tommie" Stone Sharpley. After attending the Alabama Girls Technical Institute and College for Women (now the University of Montevallo) for two years, Sharpley transferred to Auburn University in Birmingham, Alabama, as a junior in 1921. Sharpley first joined the Young Women's Christian Association at Auburn, serving as the University YWCA's president in her senior year (1922-23).

Sharpley took a job as Business and Professional program Secretary at the Baltimore, Maryland, YWCA from January 1933 through fall 1936, then moved to the national YWCA Business and Professional program staff. Between 1936 and 1944, Sharpley worked on a masters degree at Columbia while continuing her job, often part time, for the YWCA. She completed her M.A. in political science in 1944, writing her thesis on "Married Women at Work."

After World War II, the YWCA reduced and eventually eliminated its "constitutent group" work, including the Business and Professional program. Sharpley stayed with the YWCA, working as Executive Director of the Uptown Branch of the New York City YWCA (1947-49), then returning to the national staff in the Young Adult Program (1949-51). After a four-month stint as a women's affairs specialist in Germany in the summer of 1951, Sharpley returned to the national YWCA staff in Leadership Services (1952-54). She was Executive Director of the Baltimore YWCA from 1951-58.

Lilian Sharpley died in October of 1983. She is buried in Oak Hill Cemetery in Jefferson, Alabama.