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Papers of Alexander Brown relating to the writings of his books, including notes, transcripts, drafts and correspondence with publisher Houghton, Mifflin & Co. and with members of his family requesting genealogical information.

The nucleus of this collection was created from papers given to the Association by Ann Pamela Cunningham around the time of her retirement as Regent. Several other Vice Regents followed her example and later donated their papers as well. These records were referred to as the "Early Records" since the time they were first established as an archival collection. A large portion of this collection is correspondence concerning the founding of the MVLA and the operation of Mount Vernon as a historic site. Other important resources are the appeals written by Ann Pamela Cunningham and the Vice Regents, governing documents, subscription or donation lists, printed material or publications, and bound volumes such as ledgers or scrapbooks. Individual items were added to the collection as they were acquired. The Early Records includes items dated 1852-1951, however the bulk of the material dates from 1858 to around 1880.

The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Photographers primarily include staff members and contract photographers. The collection spans the 1930s to the 2000s and includes analog material made up of a variety of sizes of film negatives providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, restoration, and changes throughout the estate.

This collection contains publications concerning the history of Mount Vernon and George Washington that were not published by the Mount Vernon Ladies' Association. The MVLA collaborated with other authors and publishers to produce many of these titles, however the Association was not the copyright holder. These items have been merged together into this collection but are from different sources or accessions. Most of the publications were either originally collected by the Library at Mount Vernon, or were previously owned by Vice Regents of the Association. Others were given as gifts to the MVLA.

The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Some of the earliest photographs of the estate were created and sold to visitors by the Association as a means of income. Those efforts helped to establish an important collection of 19th century views. The collection spans the 1850s to 2000s and includes over 140 linear feet of analog material providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, and changes throughout the estate.

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.

This collection of historic manuscripts dates from 1607-1933, with the bulk of materials dating from 1738-1868. The correspondence, journals and diaries, legal and financial records, estate documents, and printed ephemera in the collection primarily relate to the Washington and Custis families, the Revolutionary War, and society life in antebellum Washington D.C. and Virginia.

Ephemera collected by Geo. Gregory Smart related to the memory and popular image of George Washington. The collection includes postcards, calendars, cigar boxes covers, stamps and first day covers, programs for anniversary events, books and pamphlets, hat stands, billheads, stationary, cartes-de-visite, playing cards, and puzzles. Some items are catchy such as a hat stand touting the motto "friends you can hang your hat on," while others are designed to be more educational such as grade-school primers or the story of the presidents from the makers of Planters peanuts.