This dataset includes rainfall, cloud, river and stream hydro-chemistry of the Plynlimon research catchments. The data is from weekly monitoring of stream hydrochemistry of the River Hafren (Severn) at both the Lower and Upper Hafren site from 1998, stream hydrochemistry of the River Hore at the Lower Hore site from 1983 and Upper Hore site from 1984 as well as rainfall hydrochemistry near the Carreg Wen meteorological site from 1983 and cloud hydrochemistry near the Carreg Wen meteorological site from 1990. Data for over 50 chemical determinands are presented alongside data for some in-situ measurements such as water temperature. Full descriptions of the analytical methods used for each determinand is included. The Plynlimon research catchments lie within the headwaters of the River Severn and the River Wye in the uplands of mid-Wales. Intensive and long-term monitoring within the catchments underpins a wealth of hydrological and hydro-chemical research; other linked datasets include river flow, meteorology and a variety of detailed spatial datasets representing the topography, soils and rivers of the catchments. Monitoring is funded by the Centre for Ecology & Hydrology, and is ongoing since 1968. Full details about this dataset can be found at https://doi.org/10.5285/44095e17-43b0-45d4-a781-aab4f72da025