The papers consist of correspondence and other materials documenting the career of Calhoun, the Calhoun and Clemson families, and United States politics during the early to mid-nineteenth century. Included are agreements, articles, clippings, correspondence, lists, notes, maps, microfilm, photographs, poems, receipts, speeches, statements, a survey book, an autograph draft and a photocopy of the South Carolina Exposition and other material.

Most of the correspondence between Calhoun and others, but other family letters are included. Some letters have been transcribed. In addition to information on the life of the Calhoun and Clemson families, topics covered by the correspondence include the condition of crops, the sale of rice, mining, the annexation of Texas, banking, construction of railroads, the Mexican-American War, nullification, presidential elections and candidates, political parties, transportation, the slavery question, state rights, and protective tariffs. The miscellaneous items in Calhoun's papers include clippings pertaining mainly to political events; handwritten copies of material relating to the slave trade in the 1790s such as an "Account of American Vessels trading for Slaves to Ye Coast of Africa"; and handwritten copies of foreign relations documents, including a summary of negotiations with Spain for the period 1816-1829, and a settlement of claims of United States citizens against Peru in the 1840s.

After Calhoun's death, correspondence and items relating to Calhoun and the papers were added to the collection. They include letters of condolence to family members following the death of John C. Calhoun; there is also correspondence pertaining to the editing of Calhoun's manuscripts pertaining to his views on government as well as letters of who should write a biography of Calhoun. The "Posthumous Miscellaneous" material includes such items as lists and indexes of Calhoun letters at Clemson by William Pinckney Starke and others; Carl L. Epting's correspondence regarding John C. Calhoun; information about Dumbarton Oaks and Fort Hill; a photograph of Fort Hill c. 1880; writings of A. G. Holmes on John C. Calhoun; and an "Order of Procession for escorting the remains of the Honorable John C. Calhoun." The "Related Material" consists of small collections of papers of other Calhoun family members kept with the Papers and includes a survey book (1784-1792) of John Calhoun's father, Patrick Calhoun; a list of John Ewing Colhoun's lands, 1789; correspondence to Floride Colhoun, 1790-1791; and the A. Ransom Calhoun papers, 1853-1862.

The maps are photostatic copies made by the South Carolina Department of Archives and History in 1976 of five maps located in Calhoun's office at Fort Hill and include a copy of a rare 1822 map of South Carolina by John Wilson. The microfilm consists of six reels of "John C. Calhoun Papers in the Library of Congress: Papers from Manuscript Groups" (Washington, DC: National Archives, 1954) and four rolls of "U.S. War Department: Records of the Office of the Secretary of War, Letters Sent, Military Affairs" for the period May 2, 1816-August 10, 1830 (File Microcopies of Records in the National Archives, no. 6, rolls 9-12. Washington, DC: National Archives, 1942).

Correspondents in the Papers include James M. Buchanan, Armistead Burt, Andrew Pickens Calhoun, Cornelia Calhoun, Floride Calhoun, James Edward Calhoun, Anna Calhoun Clemson, Thomas Green Clemson, Floride Colhoun, John E. Colhoun, Richard K. Cralle, Jefferson Davis, Carl L. Epting, James Gadsden, Duff Green, James Hamilton, J. H. Hammond, Alester Garden Holmes, Andrew Jackson, James Knox Polk, Henry William de Saussure, W. Gilmore Simms, William Pinkney Starke, Alexis de Tocqueville, John Tyler and Daniel Webster. There is a card file index to the correspondence in Special Collections.