Accurate large-scale soil moisture (SM) maps are crucial for catchment-scale hydrological models used for water resource management and warning systems for droughts, floods, and wildfires. SM can be mapped by mobile cosmic-ray neutron (CRN) systems of moderated detectors at homogeneous landscapes of similar soil and vegetation. In this study, we present a new approach for mobile CRN detection to perform to its full potential, where CRN measurements can also be converted to SM at heterogeneous landscapes. The approach is based solely on thermal and epithermal neutron datasets obtained from mobile dual-spectra CRN detection, combined with theoretical developments using a particle transport model. For each measurement point, the land cover type is identified using the thermal-to-epithermal (T/E) ratio, and the relevant neutron-count-to-soil-moisture conversion function is estimated from CRN stations located at the main land cover types in the catchment. With this approach, the requirement of collecting 100+ soil samples for each point along the survey route is omitted. We use this T/E-dependent approach to obtain SM maps from 12 CRN surveys and compare it with a simple approach where only the conversion function from the agricultural site is used. SM by the simple approach is comparable to the estimates of the agricultural stations of a capacitance sensor network, while the estimates of the T/E-dependent approach also compare well with the heathland and forest stations. With accurate SM estimates for all landcover types, the average error is reduced from 0.089 to 0.038 when comparing CRN SM with space-borne Soil Moisture Active Passive Mission estimates.