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The collection primarily contains correspondence of the Randolph family and Nicholas family. Several land title records are also present.

This collection consists of the papers of the Randolph Family of Edgehill, (commonly called the Edgehill-Randolph Papers) and the Wilson Cary Nicholas papers, ca. 787 items (6 Hollinger boxes, 2.5 linear shelf feet), ca. 1765-1869, and undated.

The papers of Anna Maria (Campbell Hickman) Otis Mead Chalmers (1809-1891) and her family offer a deep look into a 19th century American family with a sharp focus on enslaved and formerly enslaved persons. The collection documents the life of a young, widowed woman, Anna Maria Mead Chalmers, who was the granddaughter of General William Hull (1753-1825). She was a mother of four children and became a businesswoman in Richmond, Virginia. She was a writer, an editor of the Southern Churchmen, an educator and founder of Mrs. Mead's School for Young Ladies, and a director of The Southern Churchmen Cot ("Retreat for the Sick"), a hospital for children. Anna Maria's family enslaved people who are represented in the papers including Othello "Tillo" Freeman (1790's-1860's?). It includes a letter from William written in [1875], who was their carriage driver, and letters about Sam the fiddler, who settled on the farm after escaping harsher enslavement in Louisianna, and Jordan who was described as being hired out in a letter dated September 8, 1841 from Thomas R. Blair.

This collection includes correspondence between John Augustine Washington III and his mother and wife, as well as other family members, mostly dealing with family matters and running Mount Vernon.

The Bushrod Washington Family Papers consist of documents gathered by the descendants of the first President of the United States, George Washington. The collection comprises an assortment of correspondence and legal documents documenting the lives and property ownership of several branches of the Washington family. The collection is organized into five series: Correspondence, Legal Documents, Social, Miscellaneous, and Indenture Notices (Land Deeds).

The collection comprises mostly of anatomical illustrations of humans and animals by professional medical illustrators and medical practioners, but there is a good number of caricatures. Many of the images depict 20th century surgical prodedures; there are also physiological illustrations included in the collection. Most items are drawn in pencil on illustration paper with cardboard backing. In addition, there are some drawings in notepads and on tracing paper.

This collection concerns the inheritance, maintenance, and sale of the Mount Vernon estate by its last private owner, John Augustine Washington III. A large majority of the collection is correspondence to or from John Augustine Washington III with a significant portion relating to the purchase of the estate by the Mount Vernon Ladies' Association. Three diaries kept by John Augustine are also included and contain important information about his slaves, agricultural practices, and finances. Other types of material in the collection include legal documents, receipts, photographs, and ephemera. Photocopies were made for most of the manuscripts and can be viewed as surrogates to the originals.

The John L. Nau III Civil War History Collection (1806-1988, bulk 1861-1865; 133 cubic feet) contains Civil War-era correspondence, service records, pension records, artifacts, photographs, military records (including orders, requisitions, and correspondence), currency, newspapers, and other print materials.

This collection consists of letters written by and addressed to Thomas Jefferson, as well as architectural plans and studies that were created or endorsed by Jefferson, created by other individuals associated with him, deeds, plats, and maps, some of which pertain to the subjects of the architectural studies, and other miscellaneous materials.