Roloff was born in 1915 in New York City to Belle and George F. Roloff. Her paternal grandparents were from Germany. She graduated from Westfield High School. Roloff completed a B.S. from Douglass Residential College in 1937. She earned a Ph.D. from Columbia University in 1944. She was a member of Sigma Xi and Phi Beta Kappa. Her dissertation was titled, The metabolism of l(-)-pioIihe studied with the aid of deuterium and isotopic nitrogen. Rudolph Schoenheimer was Stetten's doctoral advisor.
