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A volume compiled, 1811-1830, by Thomas Llewellyn of the parishes of Cardigan and Ferwig, Cardiganshire, chiefly containing arithmetical exercises but also miscellaneous notes and memoranda in English and Welsh, perhaps partly composed by him and partly derived from printed sources. These include a bidding letter for the marriage of Mary Owen and John Williams, both of the parish of St Dogmaels, Cardiganshire, 1816; draft documents relating to property in Cardigan and Ferwig; love letters and verse in English, including a number of Valentine rhymes; prognostications in Welsh and English on the weather and on lucky and unlucky days, together with astrological notes; two apparently unpublished ballads in Welsh, one of them, perhaps by Thomas Llewellyn, recounting a case of alleged slander by Sara Evans, a Methodist, against the Rev. John Herring (1789-1832), Baptist minister at Cardigan; and a transcript of the title-page of The [Supposititious] Works of Aristotle (Arbroath, 1801) (not recorded in the Nineteenth Century Short Title Catalogue).

Papers, [1846]-1915, of Thomas Henry Thomas ('Arlunydd Penygarn') comprising correspondence, geological and antiquarian notes, translations of manuscripts and miscellanea largely of Welsh interest, including an account of the 'Mari Lwyd' and material relating to 'druidic' books and runes.

A transcript by Robert Thomas (Ap Vychan) of an extract from Edward Williams: An Essay on the Equity of Government and the Sovereignty of Divine Grace (London, 1809), and a fragment of the New Testament bearing notes of sermons preached in the Bangor district.

Copies of the coat of arms, and family tree, 1721-2008, of the Touchet and Davies families, compiled by the donor.

Two army field service books containing reports on mining operations during the fighting at Hill 60 in the Ypres Salient, 1916-17, which belonged to J. E. Jones (d. 1920), 2nd Lieut. (after Lieut.), father of the donor Olwen Caradoc Evans, together with press cuttings, 1927-1930, and photographs of him in Johannesburg.

Photocopy of Neil Sulley of the National Library of Wales's thesis 'Arolwg: ansawdd y famiaith. gwallau iaith, cywirdeb iaith, a gramadeg', submitted in partial fulfillment for the degree of BA in the Department of Welsh at University College of Wales, Aberystwyth.

Aron Elias on stage with the flag of Owain Glyndwr wrapped around his shoulders.

A file labelled, 'Diwylliant Cymru Heddiw. Celfyddyd. Wrexham. 23.11.66. Round Table/C'von. The Artist in Wales. Welsh Studies Group', containing manuscript notes of two lectures entitled 'The Artist in Wales' and 'The Fine Arts in Wales'. A list, originally inserted within the folder and later transferred to the accessions correspondence files, contains the following description of the papers: '4. Two manuscript lectures:- (a) 'Art and Meaning', (b) 'Diwylliant Cymru Heddiw'. These items were originally donated to NLW in September 1973, together with a collection of pen and ink drawings used to illustrate several books, a design for a dust jacket for the book Absalom fy Mab, pencil drawings of a bardic chair and designs for the Red Dragon of Wales (PB7959-62).

Correspondence between the donor Rosemary Markham and Peter Prendergast, Kyffin Williams, Jonah Jones, Martin Tinney and others relating to an appeal for the donation of artworks towards the exhibition 'Art for Mercy' at the Washington Gallery, Penarth, 22-24 November 2002, to raise funds for Tearfund, together with minutes of the organising committee and exhibition and auction catalogue. Also included is a letter (in Welsh), 2008, to the donor from David T. Jones, Jonah Jones's son, relating to the project 'Cofio Jonah Jones'.

Two letters, 1910-1911, from Arthur Augustine Dallman (1883-1963), secretary of the Liverpool Botanical Society and author of articles on the flora of Denbighshire and Flintshire in Journal of Botany, 1907-1911, to one Whitwell, relating to his botanical work.

A volume containing abstracts of legal cases and a dictionary of legal terms, probably compiled by Arthur Bevan, 1711.

Deeds, correspondence, pleadings and papers in legal actions, 18 cent.-20 cent., relating to estates in Anglesey, Caernarfonshire and Merionethshire. Miscellaneous papers include Caernarfon borough court rolls, 1392-1393, 1695-1697, and a rental, 1691-1692; papers relating to Benefit Building Societies in Caernarfonshire, 1861-1890; and a minute book of Porthaethwy ferry, 1782-8.

Arthur Machen's original notebook relating to The Holy Grail (1906), together with the donor's edited transcription and additional notes, 1995.

Deeds and documents, 1672-1872, relating mainly to properties in the parish of Llanfihangel Cwm Du, Brecknockshire. They also include some probate documents, extracts from parish registers and financial papers.

Papers of Robert Scourfield Mills (Owen Rhoscomyl, Arthur Owen Vaughan) and Olwen Vaughan, 1880-1977, including: works by Arthur Owen Vaughan, including genealogical notes, [1905], papers and memorabilia of National Pageant of Wales 1909, and Investiture book, 1911; letters and papers of Arthur Owen Vaughan and family, 1880-1927; newspaper articles and manuscripts concerning Arthur Owen Vaughan, 1914-1955; correspondence and papers relating to the Memorial Fund and memorial, 1921-1928; correspondence of Olwen Vaughan with relatives and friends of Arthur Owen Vaughan, 1938-1960; correspondence of Olwen Vaughan concerning the deposit of papers and other items, 1959-1970; surveys and correspondence relating to the preservation and restoration of Cherry Hinton church, Stuntney Old Hall, and Hill Hall, Essex, 1958-1968; surveys and notes on historic places in England and Wales associated with the Scourfield family, 1968-1969; and correspondence, reports and plans relating to ancient trackways in Devon and Glamorgan, 1974-1977.

Additional tranche of letters - April 2015.

Additional donation of papers and printed volumes - June 2021.