Flood risk assessment at the mesoscale requires data that are spatially and thematically detailed enough to provide reliable estimates at the catchment level. However, data availability and suitability are often contradictory: available data are rarely suitable at the required level of detail. To overcome this problem, numerous disaggregation methods have been proposed in recent decades, often based on somewhat generalised imperviousness characteristics derived from the available urban land use/land cover (LULC) nomenclature. To reduce generalisation, we propose a new disaggregation approach using a spatially distributed imperviousness density (IMD) layer at a very detailed spatial resolution of 10 m as ancillary data to improve the thematic detail of the urban classes of the available LULC datasets (Coastal Zones, Natura 2000) and the dasymetric mapping of the census data. The nomenclature of the urban classes and the impervious density thresholds were taken from the detailed Urban Atlas dataset. The disaggregation of the census data is then built on the resulting geometry of thematically improved residential classes. Assuming that IMD values indicate a built-up density, the proposed weighting scheme is IMD-dependent: it accounts for variability in the built-up density and, hence, variability in population. The approach was tested in three catchments in Croatia, each with a different degree of urbanisation. The resulting statistics (mean square error and percentage error) indicate that residential areas and population density depend on IMD. Using IMD as additional data therefore greatly improves the assessment of elements that are exposed to flooding and, consequently, the damage and flood risk assessment.