The role of soil moisture is widely accepted as a significant factor in the mass and energy balance of catchments as a controller in surface and subsurface runoff generation. The paper examines the potential of a new dataset based on advanced scatterometer satellite remote sensing of soil moisture (ASCAT) for multiple objective calibrations of a dual-layer, conceptual, semi-distributed hydrological model. The surface and root zone soil moisture indexes based on ASCAT data were implemented into calibration of the hydrological model. Improvements not only in the instrument specifications, i.e., better temporal and spatial sampling, but also in the higher radiometric accuracy and retrieval algorithm, were applied. The analysis was performed in 209 catchments situated in different physiographic and climate zones of Austria for the period 2007–2018. We validated the model for two validation periods. The results show that multiple objective calibrations have a substantial positive effect on constraining the model parameters. The combined use of soil moisture and discharges in the calibration improved the soil moisture simulation in more than 73% of the catchments, except for the catchments with higher forest cover percentages. Improvements also occurred in the runoff model efficiency, in more than 27% of the catchments, mostly in the watersheds with a lower mean elevation and a higher proportion of farming land use, as well as in the Alpine catchments where the runoff is not significantly influenced by snowmelt and glacier runoff.