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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 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.