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Payne was born in Wendover, England. In 1919, she won a scholarship to Newnham College, Cambridge University. She studied botany, physics, and chemistry. She was not given a degree because women were not given degrees by Cambridge until 1948. In 1923 she moved to the United States. She became an American citizen in 1931.
In 1933, she met Russian-born astrophysicist Sergei I. Gaposchkin in Germany. She married him in 1934.