As cities are growing in size and complexity, the estimation of air pollution exposure requires a detailed spatial representation of air pollution levels, rather than homogenous fields, provided by global- or regional-scale models. A critical input for city-scale modeling is a timely and spatially resolved emission inventory. Bottom–up approaches to create urban-scale emission inventories can be a demanding and time-consuming task, whereas local emission rates derived from a top–down approach may lack accuracy. In the frame of this study, the UrbEm approach of downscaling gridded emission inventories is developed, investing upon existing, open access, and credible emission data sources. As a proof-of-concept, the regional anthropogenic emissions by Copernicus Atmospheric Monitoring Service (CAMS) are handled with a top–down approach, creating an added-value product of anthropogenic emissions of trace gases and particulate matter for any city (or area) of Europe, at the desired spatial resolution down to 1 km. The disaggregation is based on contemporary proxies for the European area (e.g., Global Human Settlement population data, Urban Atlas 2012, Corine, OpenStreetMap data). The UrbEm approach is realized as a fully automated software tool to produce a detailed mapping of industrial (point), (road-) transport (line), and residential/agricultural/other (area) emission sources. Line sources are of particular value for air quality studies at the urban scale, as they enable explicit treatment of line sources by models capturing among others the street canyon effect and offer an overall better representation of the critical road transport sector. The UrbEm approach is an efficient solution for such studies and constitutes a fully credible option in case high-resolution emission inventories do not exist for a city (or area) of interest. The validity of UrbEm is examined through the evaluation of high-resolution air pollution predictions over Athens and Hamburg against in situ measurements. In addition to a better spatial representation of emission sources and especially hotspots, the air quality modeling results show that UrbEm outputs, when compared to a uniform spatial disaggregation, have an impact on NO2 predictions up to 70% for urban regions with complex topographies, which corresponds to a big improvement of model accuracy (FAC2 > 0.5), especially at the source-impacted sites.