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The George A. Plimpton Papers consist largely of personal and professional correspondence, financial and real estate records, personal diaries and albums, writings, and lectures produced by or for George Arthur Plimpton. But the Papers also contains not only the correspondence and records of Plimpton's colleagues at Ginn and Company, the publishing house that Plimpton led for decades, but also correspondence and records relating to the dozens of other institutions and organizations that Plimpton helped lead. In addition to extensive correspondence relating to Plimpton's collecting of rare books, manuscripts, and historical artifacts, the Papers also contain such diverse items as autographs of presidents, handwriting specimens, studies of medieval manuscripts, and documents relating to the American slave trade.

The papers consist primarily of correspondence and documentation related to her professional activities as a professor, a librarian, and a scholar of early print and book history.