The papers form 530 numbered files, and date chiefly from the end of the Second World War to the 1970s. The collection documents almost all aspects of Butterfield's academic life and writings, and provides a record of the wider development of historical studies in the course of his career.
Many of the files relate to Butterfield's historical work, especially his study of eighteenth and nineteenth century British political history, historiography and his interest in history and religion, including Christianity and history. There are drafts of Butterfield's articles, lectures, reviews and papers, and related material on these and other subjects, such as politics and science, including Butterworth's The origins of modern science. A significant part of collection is devoted to Lord Acton and the Cambridge modern history. There are correspondence and reports concerning Lord Acton, and transcripts, abstracts and notes made by Butterfield from the Acton papers in Cambridge University Library. The collection also contains correspondence and papers concerning research students and individuals, such G.P. Gooch, H.W.V. Temperley, A.J. Toynbee and Gerhard Ritter. Other subjects covered include the history of Peterhouse, Cambridge; foreign trips; invitations and visits to overseas universities; election to overseas academic positions; the British Committee on the Theory of International Politics; the receipt of honorary degrees; correspondence with historians, academics, translators and publishers; and the Dictionary of the history of ideas.
The final three files in the collection are devoted to miscellaneous correspondence. No. 529 contains letters concerning mostly academic and professional matters. No. 530 concerns mostly personal matters. No. 531 contains 497 general letters, arranged roughly in alphabetical order, the most common correspondents being G.N. Clark, G. Kitson Clark, Klaus Dockhorn, George P. Gooch, Hugh Kearney, David Knowles, Richard Koebner, Helmut Koenigsberger, T.W. Moody, Michael Oakeshott, Francis O'Gorman, George Potter, Gerhard Ritter, Karl Schweizer, Neville Temperley, Kenneth W. Thompson, G.M. Trevelyan, Adam Watson, Philip P. Wiener, Desmond Williams, G.M. Willis and Brian Wormald.