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Papers of Stuart Rendel and family members, including papers relating to the University College of Wales, Aberystwyth, and the proposal to establish the National Library of Wales and its development during the early years of its existence, 1883-1916; speeches, addresses and political papers relating to disestablishment of the church in Wales and the 1889 Intermediate Education Act, 1882-1909; press cuttings, 1881-1913; photographs, 1892; miscellaneous letters, 1878-1912; letters to Stuart Rendel, 1853-1912, including letters from A. C. Humphreys Owen, 1877-1905, family letters, 1853-1902, and letters from prominent political figures and Welsh public figures; letters and copies of letters from Rendel, 1880-1912; diaries, mainly recording details of Stuart Rendel's business activities, 1863-1869; notes of conversations with W. E. Gladstone, John Morley and H. H. Asquith, 1888-1910; papers relating to Chinese affairs and French and Chinese peace talks, 1884-1886; papers of James Meadows Rendel, including letters, 1828-1856, and papers relating to his estate, 1856-1859; letters of Catherine Jane Rendel, 1845-1855; letters and papers of George Wightwick Rendel, 1871-1902; papers relating to Rendel's other brothers, 1841-1889, and his daughters, 1882-1910; letters and papers of Harry Stuart Goodhart-Rendel, 1898-1959, and other papers concerning him, 1963-1977; papers, mainly letters, of the Goodhart family, 1819-1957; papers of Miss Rosemary Rendel, 1986-1996; papers of Sir George William Rendel, including: Foreign Office papers, 1917-1967, correspondence, 1912-1973, papers relating to the Catholic Union of Great Britain, 1942-1979, lectures, diaries and notes, 1915-1954, personal and family papers, 1908-1980, and material relating to the book The Sword and the Olive (1957), 1954-1986.

Papers of Sir Evan Vincent Evans, 1880-1933, including correspondence, 1881-1927 (comprising general correspondence to Sir E. Vincent Evans, 1881-1927, letters relating to the Ignatius Williams manuscripts, 1906-1922, drafts and copies of letters from Vincent Evans, 1893-1927, letters addressed to others, 1892-1923; and miscellaneous letters, 1894-1927, mainly those with unrecognisable signatures); bibliography of Welsh printed books, 1701-1807; minutes of the Board of Celtic Studies, 1933; records of the Diphwys Slate Quarry, 1924-1927; papers relating to education in Wales, 1887-1888; the London Committee of the Cardiff Medical Society, 1890; the National Eisteddfod of Wales, 1887-1926; the National Library of Wales, 1924-1927; the National Museum of Wales, c. 1900-1928; the Royal Commission on Ancient Monuments in Wales, 1911-1933; Royal Commission on Public Records, 1914-1916; the Society for the Promotion of Nature Reserves, 1914; the University Board of Celtic Studies, 1922-1927; the University of Wales, c. 1893-1927; the Vincent Evans Testimonial Fund, 1898-1899; and the Welsh Club, 1893-1913; together with copies of speeches and addresses delivered by Vincent Evans; and miscellaneous papers, [c. 1880]-[1930].

Press cuttings relating to Wales and Welsh culture, such as religion, politics, literature, music, education, St. David's Day celebrations and the Eisteddfod Genedlaethol, individuals, and the National Library of Wales [1895]-[1939].