The papers are a major source for British military history of the 18th century, and political, colonial, and diplomatic history of the 19th and early 20th centuries, and also contain much of interest for social history.
They fall into the following sections:
- 1. Papers of Charles, 1st Earl Grey (1729-1807)
- 2. Papers of Charles, 2nd Earl Grey (1764-1845)
- 3. Papers of Henry George, 3rd Earl Grey (1802-1894)
- 4. Papers of Albert, 4th Earl Grey (1851-1917)
- 5. Papers of Charles Robert, 5th Earl Grey (1879-1963)
- 6. Papers of Maria, Countess Grey, née Copley (d.1879), wife of 3rd Earl Grey
- 7. Papers of General Charles Grey (1804-1870)
- 8. Ponsonby Papers (John, Viscount Ponsonby, ca.1770-1855)
- 9. Cromer Papers (Evelyn Baring, 1st Earl of Cromer, 1841-1917 and his second wife)
- 10. Baring (Howick of Glendale) Papers (Evelyn Baring, 1st Baron Howick of Glendale, 1903-1973)
- 11. Copley Letters (papers of Miss E.M. Copley, sister-in-law of 3rd Earl)
- 12. Palmer Papers (Lady Sophia Matilda Palmer, comtesse de Franqueville, daughter of 1st Earl of Selborne, d.1915)
- 13. Minor members of the Grey family (chiefly Rev. Hon. John Grey (1812-95) and his daughter, and Miss Elizabeth Margaret Grey, niece of the 1st earl's wife); papers of various other family members are found among the papers of the various earls.
- 14. Grey Volumes
- 15. Grey Estate papers
- 16. Grey Pamphlets