Contains personal and professional correspondence, notes, manuscripts, offprints, lecture notes, scientific writings, records of the Astrophysical Journal, awards, honorary degrees, biographical material, photographs, and sound and video recordings. Papers span Chandrasekhar's career and document his student years at Cambridge University, his teaching career at the University of Chicago, scientific research and writing in astrophysics, editing of the Astrophysical Journal, and connections with family members and friends in India. Because of his long tenure at the University of Chicago, Chandrasekhar's papers constitute an important source for documenting the development of the Department of Astronomy and Astrophysics and Yerkes Observatory, and provide much information on colleagues and students from the late 1930s to the early 1980s. Correspondents include Lawrence H. Aller, T.G. Cowling, George Gamow, Gerhard Herzberg, Gerard P. Kuiper, Norman Lebovitz, Paul Ledoux, C.C. Lin, J.E. Littlewood, William H. Reid, Pol Swings, John von Neumann, and others. Organizations represented include the American Astronomical Society, the American Physical Society, and the Royal Society of London. Includes notes Chandrasekhar took while a student of Arthur S. Eddington, R.H. Fowler, P.A.M. Dirac and others. Also includes notes for courses taught at the University of Chicago.