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The diary, 1756-1760, of John Thomas, Tre-main, co. Cardigan, a teacher at Griffith Jones's Circulating Schools, recording his spiritual pilgrimage and including an account of his conversion experience in 1757 (ff. 33-5) as well as his soul-searching in response to some four hundred and seventy sermons by Daniel Rowland, William Williams, Howel Davies, Peter Williams, John Popkin, Richard Tibbott, William Richard and other Methodist clergy and exhorters. Also included are autobiographical notes (ff. 21 verso-5) and transcripts of letters from the hymnist Morgan Rhys (ff. 41, 87 verso-8 verso). The diary has been transcribed by John Thickens and published in Y Drysorfa, 101-3 (1931-1933) and Cylchgrawn Cymdeithas Hanes Eglwys Methodistiaid Calfinaidd Cymru, 56 (1971) and 57 (1972). Three letters, 1909, to the Reverend Gwilym Lewis, rector of Aber, co. Caernarfon, from 1925, found loose inside the volume, have been tipped in (ff. 103-8).

The collection, 1735-1778, comprises a 'short account' of Howell Harris's life, a long series of diaries, 1735-1772, memoranda, 'observations' and notes, prayers, a few letters, a note, 1742, on the differences between Howell Harris (and John Whitefield) and John Wesley, a statement, 1744, on Harris's intended marriage, extracts from diaries, spiritual observations, minutes of associations, miscellaneous memoranda and receipts, and a series of notes relating to 'affairs at Trevecka'.

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.

An autograph album belonging to Lizzie Rowlands (née Jones), Penrhyndeudraeth, Merioneth, containing entries, 1860-1911, by R. J. Derfel, Thomas E. Ellis, William Rees ('Gwilym Hiraethog'), Ebenezer Thomas ('Eben Fardd') and others including a number of prominent Calvinistic Methodist ministers; together with pasted-in photographs of some of the above and family memoranda. The album was originally owned by Lizzie Jones's father Evan Jones, London House, Bala (f. iv) and includes notes taken by him from sermons heard at Calvinistic Methodist Association and other meetings, 1847-1849 (ff. 1-6 verso). Items found loose inside the volume have been filed separately (NLW MS 22010iiE): a letter from Lizzie Rowlands, 1885, and from Thomas Charles Edwards, Bala, 1896, relating to Lizzie Rowlands's association with Mary Jones, Llanfihangel-y-Pennant, and an address by Mrs Rowlands, 1904, containing an account of the walk to Bala to purchase a Bible as recounted by Mary Jones herself.