The collection contains personal papers of Nally which trace the development of his career in the communications industry. The collection includes correspondence, photographs, and printed matter from Nally's earliest days with the Western Union Telegraph Co. (1875-1890), through his tenure with the Postal Telegraph Cable Co. (1890-1913), to his years with the Marconi Wireless Telegraph Co. of America (1913-1919); the bulk of the collection, however, covers his years with the Radio Corporation of America (RCA), for which he served as first president (1919-1923) and director, providing insight into the growth of the company, from its nascent development to its world-wide communications empire. Technological developments in radio and television (color and "ultrafax") are described, and material about the company's radio show, "The Magic Key of R.C.A.," with a script for its 1939 New Year's gala, are included.

The collection also includes correspondence, photographs, memorials, and a scrapbook of Samuel Finley Breese Morse, inventor and painter, whose great-grandfather, Samuel Finley, was the fifth president of the College of New Jersey (Princeton). Among the papers are a daguerreotype of Morse likely made by Matthew Brady about 1850 and a genealogy of the Finley and Breese families written by Morse in 1841.