The papers of Kathleen and Millicent Coleman comprise three classes of material: the private papers of the sisters and the Coleman family, 1842-1957; records relating to the National Children's Home, 1935-1981 largely CLOSED; and the Pestalozzi Village Trust, 1948-1989. Personal papers include a diary and pharmacopoeias, correspondence, examination certificates, photographs and printed books, 1842-1957, notably including a detailed manuscript medical diary describing life on board ship and a medical practice in Africa, 1842-1844, probably compiled by John Albert Sidney Coleman, grandfather of Kathleen and Millicent Coleman; pharmacopoeias containing remedies and prescriptions, with printed pharmacopoeias, compiled by Mark Coleman and others, reflecting the transition of the Coleman family business from patent remedies to modern pharmacy, 1851-1894; correspondence with Kathleen and Millicent Coleman, mainly descriptions of daily life in the National Children's Home and describing psychological testing of the children, 1927-1948 (CLOSED); family correspondence and legal documents including letting agreements and deeds of partnership, the will of Mathew Coleman, the sisters' great uncle, and relating to their father and his career, letters containing family news and gossip, 1845-1928; examination certificates and prize lists relating to the education of Kathleen and Millicent Coleman, 1922-1933; photographs of the Coleman family during the 1890s, during World War One and of Kathleen and Millicent Coleman on holiday, [1928], of Lady Eleanor Holles School, 1921-1933, group photographs of students and staff in King's College London Department of History, 1929-1955, photographs of various National Children's Home establishments, 1934-1957; a small collection of printed books concerned with the history, customs and government of London and the Home Counties, [1945-1985] (Boxes 70-74, now on open access in the Archive reading room).

The CLOSED records of the National Children's Home, 1935-1981, notably comprising Vocational Guidance Record Sheets, consisting of files on individual children that included intelligence test results, memory tests and individual comments, arranged in alphabetical order, 1938-1964 (Boxes 1-23); test results and evaluations of named children for tests organised by the National Institute of Industrial Psychology including the Porteus Maze Test and scoring sheets, 1957-1960 (Boxes 24-28); psychological evaluations of children at different branches of the children's home, notably in Cardiff, Harpenden, Nottingham and Glasgow, including individual test results and assessments with broad statistics and educational recommendations by visitors, 1942-1963 (Boxes 29-40); pupil record cards containing biographical information, aptitude tests and psychological test results for children at various homes, [1948-1960] (Boxes 41-42); material relating to the Brentwood College of Education including a working party on syllabuses, staff lists, the relationship with the University of London Institute of Education, manuscript notes and some psychological test results of children engaged in the so-called Gifted Child Study, 1971-1974 (Boxes 43-44); material relating to vocational aptitude and the placement of older children in trades and professions such as the armed forces and Civil Service, notably including psychologists' reports, 1935-1965 (Boxes 45-56); questionnaires of 18 year-old former residents conducted in 1954-1956 (Box 57); material relating to European refugees resident in the NCH including named children and correspondence with the Central Committee for Refugees, 1942-1949 (Boxes 58-59); general correspondence with Millicent Coleman relating to local authorities, staff and the emigration of children to Australia, 1951-1962; manuscript visitation report book assessing particular homes, 1946-1949; report on the incidence of enuresis (incontinence) in homes, 1946-1950; publicity material mainly created at the time of the centenary and on other children's charities, 1951-1981; careers and apprenticeship literature, 1938-1954; photographs and negatives of students and buildings, 1938-1939 (Boxes 60-62); psychological testing materials including test cards displaying words and pictures, [1958] (Boxes 63-69).

The records of the Pestalozzi Village Trust, 1948-1989, comprise typescript notes compiled by Millicent Coleman, who served on its governing Council. These consist mainly of Council minutes and supporting material, 1948-1989; Committee minutes including Finance and Management Committees, 1953-1985; Annual Reports and Accounts, 1961-1974; policy reports on the development and strategic direction of the Village, 1959-1973; correspondence with Millicent Coleman regarding Trust business and liaison with the National Children's Home, 1953-1985.

Papers of and relating to Evelyn Underhill, 1874-1997 and undated, comprising personal correspondence of and concerning Underhill, 1888-1969 and undated, the correspondents including Baron Friedrich von Hugel (three letters, 1911-1916), Underhill's husband Hubert Stuart Moore (117 letters from Underhill to Moore, 1890-1912 and undated, and 30 letters from Moore to Underhill, 1898-1906 and undated), Rabindranath Tagore (typed transcripts of 10 letters from Underhill to Tagore, 1913-1914), and members of the Underhill family, the subjects ranging from Catholicism, travels in Italy, Switzerland and France, publications and lectures, spiritual matters and advice, mysticism, health, and World War Two; correspondence, 1907-[1954], with various publishers concerning Underhill's publications (some posthumous) and broadcasts, including copyright, costs, sales and royalties; manuscripts and typescripts containing proposed holiday itineraries and recording Underhill's impressions while travelling in Italy, Switzerland and France, 1898-1899, 1901-1907; poetry, 1917-1923 and undated, including some work which was published; a speech at King's College London on being elected a Fellow, 1927; an article on 'The Fountain of Life: an iconographical study', published in 1910; material relating to spiritual development, 1921-1939, mainly under the guidance of Baron Friedrich Von Hugel and including transcripts of his letters, 1921-1924, and other items on spiritual advice, confessions, goals and progress; papers relating to retreats and religious writings, 1924-1932 and undated, including notebooks and texts of addresses; printed material by and concerning Underhill, 1926-1941, 1990, including some of her publications; press cuttings, 1891-1949, mainly reviews of Underhill's work but also including early published pieces; sketchbooks and drawings, 1892-1911 and undated, including sketches and watercolours of marine scenes in Britain, ecclesiastical subjects, and Italian and French architecture; photographs, c1925-c1930s and undated, including a photograph and negatives of Underhill (one at Pleshey), a portrait of Baron Von Hugel, marine views, and views of French and Italian castles and towns; material relating to the Underhill family, 1874-1940, including the marriage certificate of Evelyn Underhill's parents, 1874, a family tree, c1891, a copy of Evelyn Underhill's will, 1940, and details of books in Dr Williams's Library, London, which originated from Underhill's library; obituaries of and articles about Underhill, 1941-1997, including theses, bibliographies, memoirs, biographical material and reflections on her work; newsletters of the Evelyn Underhill Association, 1992-1997.