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The papers comprise correspondence files, 1918-1982, among them general and political letters to Goronwy Roberts and constituency correspondence; subject files, 1913-1981, including papers concerning foreign affairs (some deriving from Goronwy Roberts's trips abroad), domestic politics, Welsh politics and matters relating to Wales, and files of material concerning Caernarfonshire; various personalia, 1918-1982; and miscellaneous papers, 1900-1997, including printed items and press cuttings.

Papers collected by John Bryn Roberts, including correspondence, 1830-1887; legal certificates, 1863-1897; diaries, 1838-1930, kept by Bryn Roberts and some other members of the Roberts family; photographs, [c. 1880]-1924; notes on legal cases and topics, [c. 1902]-[c. 1921]; letters, 1888-1926, from John Bryn Roberts to the press; newspaper reports transcribed, 1883-1905; notes for his speeches, 1885-1905; notes on political topics, [c.1892]-[1926]; general notes, [1860]-[1894]; election addresses, 1885-1924; political leaflets and pamphlets, 1880-1927; official publications, 1889-1927; legal publications, 1863-1930; miscellaneous printed matter, 1883-1925; Calvinistic Methodist papers, 1844-1928; papers relating to the University of Wales, mainly the University College of North Wales, Bangor, 1882-1926; newspaper and magazine cuttings, 1874-1929; newspapers and periodicals, 1902-1928; bills and receipts, 1781-1926; notebooks and account books, 1833-1900.

Papers relating to the life and career of Edward Morgan Humphreys, including letters to E. Morgan Humphreys, from several prominent Welsh figures, 1900x1955, relating to professional matters, such as his articles and contributions to newspapers, requests for articles, radio talks, addresses, literary works, public appointments, his involvement with the eisteddfod and various committees; together with some letters relating to personal affairs, politics and literary matters and letters written to him in his role as an editor; miscellaneous and family ('Dyffryn') correspondence, which are mostly letters of the families of E. Morgan Humphreys' great-grandfather, the Rev Richard Humphreys, and of his grandfather, the Rev Edward Morgan, [1800]x1953; articles, radio scripts and addresses by E. Morgan Humphreys, 1902x1955; together with some personal and family papers, 1841x1955; articles, poetry, adjudications and letters to the editor of Y Genedl etc., by T. Gwynn Jones, 1890x1949; and other miscellaneous papers accumulated by E. Morgan Humphreys, [1762]x1955. Some of the family correspondence was published in 'Some Nineteenth Century Letters', in The Transactions of the Honourable Society of Cymmrodorion, 1925-1926.