Sharpey-Schafer's correspondence is extensive. In addition to his own correspondence it includes papers of William Sharpey, saved by Sharpey-Schafer after his death, 1836-70 and n.d. There are significant numbers of letters from William Sharpey himself, Sir Michael Foster, Sir John Burdon-Sanderson, Sir William Osler, George John Romanes, Sir Victor Horsley, Sir James Paget, Lord Lister, Sir Charles Sherrington, Sir William Gowers, Thomas Henry Huxley, John Newport Langley, Sir Edwin Ray Lankester, Ernest Henry Starling, Allen Thomson, Sanger Monroe Brown, Sutherland Simpson, Francis Gano Benedict, Harvey Cushing, Albrecht Kossel, Karl Hugo Kronecker, Carl Ludwig, Charles Robert Richet, and Masaharu Kohima.

Material relating to Sharpey-Schafer's career at UCL includes correspondence on his controversy in the Neurological Society with Sir David Ferrier, 1887-88, and papers relating to the rebuilding of University College Hospital in 1895.

Material relating to Sharpey-Schafer's career at Edinburgh University includes correspondence on the forced resignation of William Cramer from the department of Physiology on grounds of German nationality, 1914, and papers on the opening of the department of Animal Genetics in 1930.

Other papers reflect various aspects of Sharpey-Schafer's scientific interests, including the history of the Physiological Society (with several letters from Archibald Vivian Hill), artificial respiration and bird migration. There are also numerous letters in response to his controversial address to the British Association in Dundee in 1912, and correspondence on the position of scientists in post-Revolutionary Russia, 1918-21.

There is a substantial correspondence on the various textbooks Sharpey-Schafer wrote or to which he contributed, 1910-34.

Sharpey-Schafer's personal papers include correspondence with his wives and children, 1876-1935, scrapbooks of press cuttings, c. 1899-1930, and a large collection of photographs, mainly portraits.