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Visitor's book of Coleg Harlech, 1946-1974, including signatures of eminent people in political and cultural life in Wales and beyond who attended conferences, WEA meetings and courses at the college.

Papers of David Thomas Guy, 1912-1975, including papers relating to the Workers' Educational Association, 1920-1973, in particular of the South Wales District; minute book of Cardiff Printers Ltd, 1946-1973; papers relating to the University of Wales, 1973-1975, and Coleg Harlech, 1971-1975; papers of the Welsh Advisory Committee of the British Council, 1971-1973; appointment diaries, 1939-1973; and bibliographical notes, press cuttings, photographs and personal memorabilia, 1948-1970.

Letters, newspaper cuttings, notes, pamphlets and periodicals, typescripts, reports, volumes of parliamentary debates, and other papers of James Griffiths relating to the following: the coal industry and the South Wales Miners' Federation, 1912-1967; the Labour Party, 1919-1975; the Central Labour College, 1919-1922; National Insurance, 1931-1954; the Colonies, 1939-1972; his work as Secretary of State for Wales, 1964-1966; papers relating to Welsh affairs including devolution, the Welsh Reconstruction Advisory Council, education and local government reorganization, 1935-1975; constituency affairs, 1937-1969; overseas visits, 1936-1968; the Nigeria-Biafra War, 1968-1970; papers relating to his autobiography Pages from Memory, including letters from Gwilym Prys Davies and others, 1961-1969, notebooks, [1960s], typescripts, [1964]-1969, and cuttings of reviews, 1969; unpublished reminiscences, 1955-1974; notes and typescripts for lectures and speeches, 1940-1971; typescripts of broadcasts by Griffiths, 1937-1967; typescripts of articles and reviews, 1940-1974; newspaper cuttings, 1919-1974; and other miscellaneous personal matter, [1930s]-1975; and papers relating to Mrs Silyn Roberts, 1897-1954.

Papers and correspondence of Robert Silyn Roberts and his wife Mary Silyn Roberts, 1888-1965, including correspondence 1904-1965, including papers relating to the establishment and early development of Coleg Harlech, 1926-1928.

Papers of Sir Ben Bowen Thomas (1899-1977), educationalist and public servant, comprising autobiographical material on his career, interests and family, 1954-1972; biographical articles and an interview, 1964-1966; letters to his wife and daughter with references to his work with UNESCO and Welsh educational matters, 1947-1960; letters from Dr Thomas Jones and Sir Percy E. Watkins relating to educational issues and Coleg Harlech, 1926-1955; correspondence concerning BBT's work with UNESCO, 1954-1962; miscellaneous correspondence, 1948-1976; addresses and speech notes, 1949-1977; pamphlets, offprints and articles, 1941-1973; research notes on regions and towns of Wales during the 18th and 19th centuries; circulars, articles, reports, etc. relating to education and educational bodies in Wales, 1942-1975, to UNESCO, 1946-1958, and to public and cultural bodies such as the Welsh Language Council, ITA and the Rural Development Board, 1965-1973; McNair Report on the Training of Teachers, 1942-3; memorials, tributes and obituaries of other educationalists; and miscellaneous press cuttings and notes. The archive also includes a collection of sermon notes and exercise books of his grandfather, the Rev. Benjamin Thomas, (1838-1913), a Baptist minister in Ystrad Rhondda, Glamorgan.