Using the railway system for regular environmental monitoring could extend the measurement capability to trans-regional and nationwide scales. Cosmic-ray neutron detectors in trains respond to spatial patterns of water content in their environment. Three distinct real world experiments support a proof of concept for soil and snow water monitoring using trains on short and long-range tracks across Germany: Supplement S4: Data (raw and processed) for the train journey from Leipzig to Berlin. Supplement S5: Data (raw and processed) for the train journey from Dessau to Zerbst, the subsequent car-borne Rover measurements, and the TDR measurements. Supplement S6: Data (raw and processed) for the train journey from Garmisch-Partenkirchen to Munich to Leipzig. This is the dataset supplementing the corresponding GRL publication "Neutrons on Rails -- trans-regional monitoring of soil moisture and snow water equivalent", preprint available from: https://doi.org/10.1002/essoar.10507363.1

We acknowledge German Weather Service (DWD) for air humidity and temperature data and the NMDB database (www.nmdb.eu), founded under the European Union's FP7 program (contract 213007) for providing data for incoming radiation from the Jungfraujoch monitor (Physikalisches Institut, University of Bern). Funded by DFG (German Research Foundation) via the project 357874777, research unit FOR 2694 Cosmic Sense; infrastructural funds of the Helmholtz Association, the Terrestrial Environmental Observatories (TERENO), and Modular Observation Solutions of Earth Systems (MOSES).