Eleuthera du Pont Smith's papers consist primarily of correspondence, both incoming, dating from 1831 to 1876, and outgoing, dating from 1816 to 1875. They contain discussions of family news, sewing, domestic activities, and travels in the United States and Europe.

The papers also include Eleuthera's diaries from 1840 to 1874, though incomplete. They contain descriptions of fancy sewing and visiting, as well as church attendance, with the subjects of sermons, lists of gifts given and received, and operations of the Brandywine Manufacturers' Sunday School. An account book from 1870 to 1874 contains expenses such as servants' wages and donations to churches, the American Missionary Society, and the Sewing Society. The papers also include a journal of an 1829 trip to Philadelphia, New Jersey, and New York and another of a European trip from 1846 to 1847.

Eleuthera's miscellaneous papers include family genealogical notes; extracts from the writings of Du Pont de Nemours, Victor du Pont, and Turgot; an account of the death of Alexis I. du Pont; a list of visitors to Eleutherian Mills (including Lafayette); and notes on the Maréchal de Grouchy. Her autograph collection materials are also in this part of the collection. Much of Smith's autograph collection was given to her by General Mercier du Paty de Clam, a son of Adrien Mercier du Paty de Clam, and his wife, Marie Jacqueline Bidermann, with each item certified by him. Sketchbooks contain various drawings, including scenes along the Brandywine, birds, flowers, and caricatures. Ten volumes of school copybooks include history, geography, poetry, and literature. There are also examples of poetry, recipes, prayers, devotions, and copies of sermons.

Dr. Thomas MacKie Smith's papers include letters written to Eleuthera while she was away, describing domestic life in her absence. His papers also include a medical account book from 1833 to 1851 and a record of babies delivered from 1834 to 1852.