The collection consiste of correspondence, memoranda, reports, bulletins, clippings, photographs, awards, and printed material. The files, arranged by genre and topic and reflect her philanthropic and legislative work in the areas of health, specifically cancer, heart disease, and mental health. Her civic and legislative work is covered in detail, as well as her private interests and activities.

Correspondence, memoranda, photographs, manuscripts, lists, legal and financial documents, and printed materials of Simon. The personal and business papers include correspondence with authors, inscribed photographs of authors, editorial files, files for his special art, photography, and music projects, correspondence files relating to Simon and Schuster, Inc., personal and family correspondence, documents, and photographs. Correspondents include Irving Berlin, Margaret Bourke-White, Henri Cartier-Bresson, Joseph E. Davies, Dwight D. Eisenhower, Philippe Halsman, Jerome Kern, Cole Porter, Kenneth Roberts, Arthur Schnitzler, Jerome Weidman, and Sloan Wilson.