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Papers of Smedley, including correspondence, memoranda, manuscripts, and printed materials about the United Nations, national politics and elections, and civic organizations in New York City and in Connecticut. Correspondents include Hubert Humphrey, John F. Kennedy, and Bertrand Russell.

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.