This dataset contains daily and sub-daily hydrometeorological and soil observations from COSMOS-UK (cosmic-ray soil moisture) monitoring network from October 2013 to the end of 2017. These data are from 46 sites across the UK recording a range of hydrometeorological and soil variables. Each site in the network hosts a cosmic-ray sensing probe; a novel sensor technology which can be used, in combination with hydrometeorological data, to calculate the volumetric water content of soil over a field scale. The hydrometeorological and soil data are recorded at a 30 minute resolution and they include neutron counts from the Cosmic-ray sensing probe, humidity and atmospheric pressure data that are used to derive volumetric water content at two temporal resolutions (hourly and daily). Also included are soil heat flux, air temperature, wind speed and radiation data which are used to derive potential evapotranspiration at a daily resolution. This work was supported by the Natural Environment Research Council award number NE/R016429/1 as part of the UK-SCAPE programme delivering National Capability.