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The collection includes Schiller's notebooks, his working notes, scripts of his lectures, articles and essays, correspondence concerning engagements and with colleagues and students, material relating to his involvement with courses for teachers, personalia, printed material and photographs. Schiller's notebooks mainly contain working notes and the text for his lectures which provide evidence of his educational ideas, for instance, on the teaching of numbers, the importance of freedom and creativity through art, craft and movement activities, on reading, writing and conversation.
Also included are the notes and papers of Schiller's wife, Mrs Lyndall Schiller, including diaries of their daughters' childhood development. These records of Lyndall were deposited along with those of her husband and as much of them relate to matters that were of interest to both of them they have been retained within the collection of her husband's papers.
In addition the collection contains papers of two of Schiller's students who attended the 'Course on the Education of Children in the Junior School' organised by Christian Schiller at the University of London Institute of Education, 1959s. These include some wooden mathematical teaching apparatus.

Papers of the Board of Education Inspectors' Association (later the Association of Her Majesty's Inspectors of Schools), 1871-1992, including annual reports, minutes and papers of the Executive Committee and Divisional Committees, reports and memoranda, 1920-1992; lists of Divisions, Districts and staff, issued by the Education Department, 1871-1946; collected personal papers of individual HMIs; material gathered for a post-war history of the Inspectorate.

The Katherine Bathurst Papers, 1891-1932, focusing mainly on her career at, and disputes with, the Board of Education, her interests in nursery education, the working conditions of the school inspectorate and the position of women within the inspectorate. The papers comprise inspection notes from school visits; notes for her preliminary and supplementary reports; copies of Board of Education Circulars; photocopies of the Women Inspectors' Reports; correspondence with her superiors and officials at the Board of Education; private correspondence, including with Sir John Gorst; correspondence with the National Union of Women Teachers (NUWT) and National Union of Teachers (NUT); published and unpublished articles; education pamphlets; and newspaper clippings of articles and editorials related to her dispute with the Board of Education and on general educational topics.