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The biographical series contains information about James M. Buchanan's personal life, education, awards, and clippings of articles about him and his career. There are also materials kept by his wife, Ann Bakke Buchanan. The series is divided into four subseries: Ann Bakke Buchanan papers, Education, Awards, and Clippings. Additional materials not in subseries include personal photographs and Buchanan family history.

The correspondence series contains letters, emails, memoranda, cards, and other forms of written communication sent to and received by Buchanan. The series is divided into two subseries: alphabetical correspondence and chronological correspondence. The bulk of the correspondence was filed alphabetically by correspondent or type of correspondence. A small amount of unrelated correspondence was grouped together in date ranges, likely by either Buchanan himself, or his assistants Betty Tillman and Jo Ann Burgess. The bulk of the correspondence in both subseries deals with Buchanan's professional career from his time at the University of Virginia until his retirement, including discussion of publications, manuscripts, events, and academic business. The bulk of the correspondence starts in 1950. There are very few letters prior to 1950. There is a photocopy of a letter from 1941 in Box 56 Folder 1 J.

The writings series contains drafts, typescripts, photocopies, notes, and reprints of Buchanan's books, articles, speaking lectures, and unpublished material. There are also research files relating to some of his writing projects, and some correspondence with publishers, coauthors, and reviewers. The series is filed alphabetically by title of the work. Note that some of Buchanan's works went by multiple titles in the draft stage, and may not be filed together as a result. Some papers presented by Buchanan at conferences or given as lectures are located in Series 5: Professional services Subseries 1: Conferences and events.

This series contains materials relating to Buchanan's work at various universities, notably University of Virginia, Virginia Polytechnic Institute (VPI or Virginia Tech), and George Mason University. The series is divided into five subseries: Administration, Teaching, Grants, Thomas Jefferson Center for Studies in Political Economy, and Center for Study of Public Choice.

This series contains materials relating to Buchanan's professional activities outside of his university and Center for Study of Public Choice responsibilities. The series is divided into two subseries: Conferences and events, and Consulting and organizations. The series is arranged chronologically.

Betty Tillman was an administrative assistant for James M. Buchanan and the Center for Study of Public Choice from 1962 to 2007. Her work included typing Buchanan's correspondence, scheduling his travel and conference events, and liaising with publishers and outside parties on Buchanan's behalf. As a member of the Center and eventual administrative director, she made arrangements for the visiting scholars program, managed personnel, kept financial records, and coordinated events and conferences, among many other duties. As her work was integral to Buchanan's and the Center, her papers are somewhat integrated with Buchanan's and the Center papers as well. In the course of processing, some of her papers were able to be identified as a discrete series.

Jo Ann Burgess was an administrative assistant at the Center for Study of Public Choice from 1989 to 2014. She was responsible for the library at the Center and for the management of Buchanan's papers. Additionally, she was the secretary for the Public Choice Society and edited much of Buchanan's published works in the 1990s and 2000s, notably The Collected Works of James M. Buchanan, published by the Liberty Fund. As her work was closely tied to Buchanan's and the Center, her papers are somewhat integrated with Buchanan's and the Center papers. In the course of processing, some of her papers were able to be identified as a discrete series.

This series contains articles, books, and other writings by authors other than Buchanan. Some materials have notes and annotations. Some materials contain correspondence with the authors. Some writings are about Buchanan and his ideas. Some writings were filed by author, others were in folders containing writings from multiple different authors. No additional filing out of writings was done under the NEH grant. The series is arranged alphabetically by surname of author. Materials where Buchanan is a coauthor are found in Series 3: Writings.