Links between forest floor carbon:nitrogen (C:N) ratios, atmospheric N deposition and nitrate leaching into surface waters have been reported for forest ecosystems, but similar studies have not been reported previously for the equivalent compartments of moorland ecosystems in Great Britain, despite the importance of nitrate in contributing to the acidification of moorland streams and lakes in British uplands. In this paper, the relationships between the C:N ratio of moorland soil surface organic matter, N deposition, and nitrate leaching are explored for 13 soils in four moorland catchments. Although there is spatial variability in the C:N ratio of soils, major differences are apparent between soils and especially between catchments. The C:N ratio appears to be inversely related to modelled inorganic N deposition and, to a lesser degree, measured nitrate leaching, for three of the four catchments studied (Allt a'Mharcaidh, Afon Gwy, and Scoat Tarn). Nitrification may make an important contribution to nitrate leaching at the two higher deposition sites. At the fourth site, the heavily acidified River Etherow catchment, extremely high rates of nitrate leaching are not accompanied by low C:N ratios or high nitrification potentials in the upper soil horizons. Hence the C:N ratio of surface soil organic matter may have potential as an indicator of nitrogen saturation and leaching in some systems, but it is not universally applicable.