Subseries1, Government Service Correspondence, 1951-1969, includes correspondence from Bundy's time in government service positions. This includes the Central Intelligence Agency, Department of Defense, and Department of State. The bulk of the materials are letters of congratulation and farewell for his appointments as Deputy Assistant Secretary of Defense for International Security Affairs (1961-1963), Yale University Trustee (1961-1980), Assistant Secretary of Defense for ISA (1963-1964), and Assistant Secretary of State for East Asian and Pacific Affairs (1964-1969). The Department of State memoranda cover topics such as McNamara and Taylor's Mission to South Vietnam, Vietnam Press Releases, Southeast Asia, and military and political policies in Vietnam. The CIA correspondence documents relate to Bundy's subpoena and testimony in the McCarthy Loyalty Review Board and his relationship with Alger Hiss. Many are letters of outrage that the charges were brought against Bundy. Some felt that McCarthy was striking at Dean Acheson and Allen Dulles through Bundy. Also included is the statement that Bundy gave to the Loyalty Board Panel. He was eventually cleared of all charges by Allen Dulles, the then CIA Director.

Correspondence in this subseries is arranged alphabetically and the Department of State memoranda are arranged chronologically.

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Subseries 2, Foreign Affairs Quarterly Correspondence, 1971-1984, contains correspondence from Bundy's tenure as editor of Foreign Affairs from 1972 to 1984. This correspondence includes letters and a small number of manuscripts from ambassadors, politicians, government officials, academics, and the media and is arranged alphabetically by correspondent's last name. Bundy corresponded with people from around the world, including Germany, Switzerland, Israel, Japan, Pakistan, Poland, France, China, and Great Britain, with some letters written in French of Chinese. Correspondence can be found from the National Security Council and the House of Representatives Committee on Foreign Affairs and from research institutions, such as The Brookings Institution, and The International Institute for Strategic Studies.

Several topics prevailed during Bundy's tenure as editor, including NATO diplomacy and military strength, SALT I, SALT II, terrorism, Iran and the hostage crisis, OPEC, world economics, Chinese-U.S. relations, Japan, the Middle East, and global fuels and energies. Letters on these topics and other interests can be found from George Kennan, Paul H. Nitze, Louis Halle, Clark Clifford, and George W. Ball. However, there is very little mention of African issues in this collection despite the numerous articles found in the journal. Also, several authors whose articles appear in the journal are absent from Bundy's correspondence. Additionally, a small amount of inter-office memoranda discussing journal business is also found.

Correspondence in this subseries is arranged alphabetically.

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Subseries 3, General Correspondence, 1961-2000, contains personal correspondence between family, friends, domestic and international contacts, authors, and political leaders. Includes a large amount of letters to authors of books Bundy read and critiqued. In particular, Bundy was heavily involved in the controversy concerning the 1975 publication of Bodyguard of Lies by Anthony Cave Brown. Brown challenged the loyalty of Prince Bernhard of the Netherlands in the ULTRA-operation (from 1940, the system by which much of the German military wireless traffic was secretly decoded by the British). Additional records and correspondence regarding the controversy can be found in the Series 2, Subject Files. Letters also reveal the personal relationships Bundy had with friends over the years. This includes his long-time relationship with Stuart Milner-Barry who served with Bundy at Bletchley Park in England. Correspondence relating to Bundy's book A Tangled Web is in Series 8.

Correspondence in this series is arranged alphabetically.

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Subseries 1, Tangled Web, 1961-2000, is divided into three sections: general, correspondence, and subject files. The first section includes the outlines, notes, and reviews. Section two contains the major correspondence Bundy had concerning the book. Major correspondence is between Marshall Green, Winston Lord, and Kent Sieg. The third section is made up of subject files that Bundy compiled while researching his book. The subjects include major issues regarding foreign policy during the Nixon presidency such as Cambodia, the Chennault Affair, Iran, the Middle East, Paris Negotiations, and Vietnam. The CIA files contain copies of intelligence memorandums, information cables, and special reports. Many of the files also include copious notes Bundy drafted as he reviewed the documents.

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Subseries 2, Articles and Miscellaneous Writings, 1965-1997, contains articles, essays, book reviews, forewords, introductions, columns, and personal poetry. Bundy produced numerous articles during his lifetime for various foreign and domestic publications and various editorials for Foreign Affairs. He tackled topics such as national security and government service, with the bulk of articles examining U.S. foreign policy toward Vietnam. During the early 1970s, Bundy wrote a guest columnist series for Newsweek. These articles focused largely on foreign policy and examined such issues as the Nixon doctrine, the Middle East, and Vietnam. The series also includes a large manuscript about Vietnam that Bundy wrote immediately after leaving the Department of State in1969. Bundy utilized his classified papers and files, which he could not cite at the time. With the Pentagon Papers and other documents coming to light, he never went back and made the necessary citations. Thus, the manuscript remains in an incomplete state, but still reveals a great deal of research concerning Vietnam foreign policy.

The writings in this subseries are arranged by type, including articles, book reviews, essays, introductions, letters to the editor, columns, poetry and miscellaneous.

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