Correspondence, memoranda, minutes, speeches, writings, interview transcripts, reports, research files, calendars and schedules, financial and legal records, travel files, academic records, biographical material, childhood diaries and writings, family papers, honors and awards, scrapbooks, printed matter, electronic files, cartoons, photographs, and other papers documenting Greenfield's career in journalism as Washington correspondent and editor for Reporter magazine (1961-1968), editorial writer and editor of the Washington Post editorial page (1968-1999), and columnist for Newsweek (1974-1999). Also documents her studies at Smith College and the University of Cambridge, years in Rome (1952-1955), work for Adlai E. Stevenson's 1956 presidential campaign, and membership on the Pulitzer Prize Board. Subjects include New York state and national politics, foreign policy, public policy, science policy, U.S. Congress, civil rights, the Vietnam War, political culture and social life of politicians, social life in Washington, D.C., and Greenfield's Pulitzer Prize for editorial writing. Writings include drafts of her memoir, Washington, which was completed and posthumously published in 2001 by Michael R. Beschloss.

Includes interviews with Marion Barry, Jimmy Carter, Nicolae Ceauşescu, Jeremiah A. Denton, Louis Farrakhan, Hamilton Jordan, Walter F. Mondale, George Pratt Shultz, William H. Webster, Caspar W. Weinberger, and Anne L. Wexler; and notes from Max Ascoli, Benjamin C. Bradlee, Leonard Downie, and Donald E. Graham.

Family papers include correspondence, genealogical material, photographs, and testimony of Lorraine Nathan Greenfield in the murder trial of Nathan Freudenthal Leopold and Richard A. Loeb in 1924. Family correspondents include Greenfield's parents, Lewis J. Greenfield and Lorraine Nathan Greenfield; brother, Jim Greenfield; and other Greenfield and Nathan family members.

Correspondents include Dean Acheson, Joseph Alsop, Nancy Kassebaum Baker, Russell Baker, George W. Ball, Leonard Beaton, Christopher Buckley, William F. Buckley, Warren Buffett, George Bush, Bruce Kerry Chapman, Daniel Ellsberg, Nora Ephron, Bill Gates, Melinda Gates, William H. Gates, Robert Gottlieb, Fred Charles Iklé, Lady Bird Johnson, Alfred Kazin, Slim Keith, Larry L. King, Irving Kristol, James Lehrer, Nicholas Lemann, Anthony Lewis, Anne W. Marks, Mary McGrory, Daniel P. Moynihan, Anne L. Wexler, Tom Wicker, and George F. Will.