The first NPG director, Charles Nagel, was appointed in 1964. Most of the records document the director's efforts to initiate programs to fulfil the second mission of the Gallery: to provide a research center for American biography, iconography, and history. To achieve this objective, Charles Nagel established the Catalogue of American Portraits and the Charles Willson Peale Papers. During his tenure, Nagel acquired additional small collections such as a few Andrew Mellon portraits and transfers from the National Museum of History and Technology and the National Collection of Fine Arts. Also, the records document NPG's move from the Arts and Industries Building in 1967 to its present quarters in the Old Patent Office Building.
Records for the tenures of Marvin Sadik and Alan M. Fern mostly document major programmatic innovations, such as the Living Self-Portrait and Portrait in Motion series, that resulted in colloquia. The records also document special exhibition schedules, the donation in 1974 by Paul Mellon of 761 engraved portraits by C. B. J. F. de Saint-Memin, the donation by Time Incorporated of 850 pieces of art used on Time magazine covers, and 5,419 glass negatives from the Mathew Brady Studio, which were acquired in 1981 from the Frederick Hill Meserve Collection.
Included in the records are internal correspondence between the directors and NPG staff; correspondence with other Smithsonian bureaus as well as with other local, national, and international art institutions and artists; and numerous public inquiries about artists, works of art, exhibitions, donations of art, and bequests. These records also include color and black and white photographs, color slides, exhibition designs, exhibition materials such as catalogues, installation photographs, check lists, names and addresses of financial and art donors, shipping and loan forms, insurance forms, reports concerning the security of the collections and the Gallery, and condition reports that mostly document loan exhibitions and some new acquisitions. There are also minutes from various committee meetings within and outside NPG.