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The collection includes journals, correspondence, poems and juvenilia by Macaulay, notes made in the course of his historical research, a scrapbook of broadsheet ballads kept by him, financial papers, and material relating to the publication of his works. There is a substantial amount of material relating to Macaulay's executors' administration of his estate, including the sale of his house, Holly Lodge, as well as correspondence regarding a dispute with Macvey Napier in 1875 over the publication of letters by Macaulay.

Papers of other members of the Macaulay family are also linked, including diaries of Zachary Macaulay in the West Indies and Sierra Leone (1795-1798) and a diary of Kenneth Macaulay in Sierra Leone (1809-1911), as well as a memoir of her brother by Hannah More Trevelyan and an album of poetry kept by her.