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Cosmic-ray neutron sensing (CRNS) has become an effective method to measure soil moisture at a horizontal scale of hundreds of metres and a depth of decimetres. Recent studies proposed operating CRNS in a network with overlapping footprints in order to cover root-zone water dynamics at the small catchment scale and, at the same time, to represent spatial heterogeneity. In a joint field campaign from September to November 2020 (JFC-2020), five German research institutions deployed 15 CRNS sensors in the 0.4 km2 Wüstebach catchment (Eifel mountains, Germany). The catchment is dominantly forested (but includes a substantial fraction of open vegetation) and features a topographically distinct catchment boundary. In addition to the dense CRNS coverage, the campaign featured a unique combination of additional instruments and techniques: hydro-gravimetry (to detect water storage dynamics also below the root zone); ground-based and, for the first time, airborne CRNS roving; an extensive wireless soil sensor network, supplemented by manual measurements; and six weighable lysimeters. Together with comprehensive data from the long-term local research infrastructure, the published data set (available at https://doi.org/10.23728/b2share.756ca0485800474e9dc7f5949c63b872; Heistermann et al., 2022) will be a valuable asset in various research contexts: to advance the retrieval of landscape water storage from CRNS, wireless soil sensor networks, or hydrogravimetry; to identify scale-specific combinations of sensors and methods to represent soil moisture variability; to improve the understanding and simulation of land–atmosphere exchange as well as hydrological and hydrogeological processes at the hillslope and the catchment scale; and to support the retrieval of soil water content from airborne and spaceborne remote sensing platforms.