Climate change increases the occurrence and severity of droughts due to increasing temperatures, altered circulation patterns, and reduced snow occurrence. While Europe has suffered from drought events in the last decade unlike ever seen since the beginning of weather recordings, harmonized long-term datasets across the continent are needed to monitor change and support predictions. Here we present soil moisture data from 66 cosmic-ray neutron sensors (CRNSs) in Europe (COSMOS-Europe for short) covering recent drought events. The CRNS sites are distributed across Europe and cover all major land use types and climate zones in Europe. The raw neutron count data from the CRNS stations were provided by 24 research institutions and processed using state-of-the-art methods. The harmonized processing included correction of the raw neutron counts and a harmonized methodology for the conversion into soil moisture based on available in situ information. In addition, the uncertainty estimate is provided with the dataset, information that is particularly useful for remote sensing and modeling applications. This paper presents the current spatiotemporal coverage of CRNS stations in Europe and describes the protocols for data processing from raw measurements to consistent soil moisture products. The data of the presented COSMOS-Europe network open up a manifold of potential applications for environmental research, such as remote sensing data validation, trend analysis, or model assimilation. The dataset could be of particular importance for the analysis of extreme climatic events at the continental scale. Due its timely relevance in the scope of climate change in the recent years, we demonstrate this potential application with a brief analysis on the spatiotemporal soil moisture variability. The dataset, entitled “Dataset of COSMOS-Europe: A European network of Cosmic-Ray Neutron Soil Moisture Sensors”, is shared via Forschungszentrum Jülich: https://doi.org/10.34731/x9s3-kr48 (Bogena and Ney, 2021).