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Fonds documents the Mallochs' activities related to their medical and literary work. The fonds contains notes, correpondence, commonplace books, account books, material related to publications, family memorabilia, scrapbooks, photographs, telegrams, postcards and certificates.

The Sir William Osler Collection, distinct from the Bibliotheca, is an extensive archival holding of Osler's correspondence (including eighteen hundred original letters), daybooks, accounts, engagement books, legal documents, book invoices, membership certificates, notebooks, lectures, addresses, newspaper clippings, photographs, books with manuscript additions, and miscellaneous loose items formerly inserted into individual books in his library. The collection also contains various family papers, including correspondence of Lady Grace Revere Osler and Edward Revere Osler.