Letters, mainly to John Roberts and Samuel Roberts from Mary Davies, Kerry School, 1834; Evan Evans, Aberrhiw, 1822 (with a 'cywydd' entitled 'Sylwadau y Bardd pan glywodd farw y Parchedig George Lewis, D.D.'); Henry Tobit Evans, Aberystwyth (Michael D. Jones testimonial), 1881; James Griffiths, Lanveran, 1816; Thomas J. Griffith, Utica, 1877; William Hughes, Dolgelley, 1870; Morris C. Jones, Welshpool, 1875; Tomos D. Jones ('Rhodwy'); Jenkin Lewis, Newport, 1819; D. Richards, South Petherton, 1828, Evan and Betty Roberts, Tan-y-ffordd, 1812, with a draft letter by John Roberts, Diosc; George and Jane Roberts, Ebensburg, 1844-1845; John Roberts, Llanbrynmair (to Jenkin Lewis, Newport), 1815; (to Mr. James of Abergavenny, 1824, (to David Richards, South Petherton), 1831-1834; Samuel Roberts (to Edward Davies, Newtown), 1829, (to Mrs. Yallowley), 1829, (to Lord Aberdare), 1875; John Turner Stannard, Huddersfield, 1884; Richard Tibbott, Llanfyllin, 1834; R. D. Thomas ('Iorthryn Gwynedd'), Knoxville, 1875; Richard Williams, Celynog, 1875; and Sarah Yallowley, Bryn-y-gyn; 'Gogan-gerdd Ynys Prydain' and an incomplete account of Tennessee by 'Gruffydd Rhisiart'.

Holograph manuscripts of essays, articles and addresses by Samuel Roberts ('S.R.'):- 'Address on behalf of Sabbath Schools'; 'Adgofion Cymru, y Gymraeg, a'r Cymry'; 'Rhai o'r siomedigaethau a'r Trallodion a welsom yn Tennessee'; 'Cynghorion i Athrawon yr Ysgol Sabbothol'; and 'Cynghorion i gyfansoddwyr ieuanc'.

Notes of Samuel Roberts ('S.R.')'s preparations for journeys in the United States, 1860-64; notes on conditions in Tennessee during the Civil War and a list of damages suffered by Samuel Roberts; a short essay on the decline of trade in America; and a printed petition by 'S.R.' to the Accounting Officer of the Treasury Department at Washington, D.C., 1881.