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Llangibby Castle estate records, including court rolls of manors in Monmouthshire, 1262-1911, Glamorgan, 1675-1739, Gloucestershire, 1427-1595, and Somerset, 1609-1691; title deeds, mainly Monmouthshire, 1217-1930, and correspondence, mainly 18-19 cent.; important letters and papers relating to the civil war in Monmouthshire; and manuscripts aquired by the family, including drafts and copies of Modus Tenendi Parliamentarum and Observata Parliamentaria by Henry Elsynge, junior (1598-1654), clerk to the House of Commons, together with minutes of the House of Commons, 1624-1626, calendar of the Journal of the House of Lords, 1647-1768, copies of the Journals of the House of Commons, 1547-1701, index to parliamentary proceedings, temp. Edward III-Edward IV, and, 1724-1743, civil war tracts, the journal of the missionary Dr Joseph Wolff, 1832, 'Prif Achae holh Gymru Benbaladr' in the autograph of Sir Thomas Wiliams, Trefriw, 1578-1609, a seventeenth-century collection of Welsh poetry by the principal 'cywyddwyr'; a memoir of Richard Robert Jones ('Dic Aberdaron', 1780-1843) in his own autograph; English sermons and miscellaneous notes by Rev. Edmund Jones, Pontypool, a sermon notebook of Rev. Philip Henry (1631-1696), the eminent Nonconformist divine, a survey of the lands of Henry, earl of Pembroke, in Glamorgan and Monmouthshire, 1570, and a survey of lands in the lordship of Usk, 1619; pedigree rolls of Sir Roger Williams of Penrhos, Monmouthshire, compiled by Thomas Jones ('Twm Siôn Catti'), 1591, and of the Williams family of Llangibby Castle, probably compiled by Sylvanus Morgan.

Manuscripts, [late 12 cent.]-[early 20 cent.], formerly part of the library of the Mostyn family of Mostyn Hall, Flintshire, comprising transcripts and extracts from Giraldus Cambrensis, Geoffrey of Monmouth, Dares Phrygius, Nennius, Gildas, David Jenkins (Judge Jenkins), Sir John Wynn of Gwydir, Lydgate's 'Life of Our Lady', Leland's Itinerary, 'Chroniques de France', historical manuscripts such as Brut y Tywysiogion and Brut y Brenhinoedd, Welsh romances and the Mabinogion; collections of mainly Welsh poetry, among them the seventeenth-century volumes Llyfr Coch Nannau and Llyfr Gwyn Corsygedol, containing poems by Dafydd ap Gwilym, Guto'r Glyn, Tudur Aled, Siôn Cent and others; genealogies, pedigrees and histories; official papers relating to Caernarvonshire; catalogues of the Mostyn and Gloddaeth libraries, 1692-1842; etc.

Papurau W. J. Gruffydd,[1903]-[1952], yn cynnwys drafftiau o erthyglau'n ymwneud â'r Mabinogi; nodiadau darlith ar gyfer ei gyrsiau Cymraeg yng Ngholeg Prifysgol Cymru, Caerdydd; nodiadau darlithoedd ac erthyglau eraill; sgyrsiau a darlledwyd gan y BBC; personalia; a grŵp sylweddol o ohebiaeth oddi wrth ffigurau llenyddol blaenllaw = Papers of W. J. Gruffydd, [1903]-[1952], including drafts of articles relating to the Mabinogi; lecture notes for his Welsh courses at University College of Wales, Cardiff; other lecture notes and articles; BBC broadcast talks; personalia; and a substantial group of correspondence from notable literary figures.