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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.

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.

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.

Papurau gan gynnwys llythyr oddi wrth Percy E. Watkins, 1926, yn ymwneud â sefydlu'r Coleg; llyfr cofnodion y Gymdeithas Gymraeg, 1931-1938; llyfryn Horace Haigh, myfyriwr yn y Coleg, 1936-1937; amserlen, 1947-1948; llyfr nodiadau darlithiau Llên Gymraeg, [1947]-[1948], ynghyd â nodiadau dosbarthiadau diweddarach, 1962-7; prosbectws cyrsiau 1946-1947; Adroddiad Blynyddol, 1949-1950; a Y Bont (Cylchgrawn Coleg Harlech, 1954-1955).