Emissions of CO 2 from road vehicles were 1.57 billion metric tons in 2012, accounting for 28% of US fossil fuel CO 2 emissions, but the spatial distributions of these emissions are highly uncertain. We develop a new emissions inventory, the Database of Road Transportation Emissions (DARTE), which estimates CO 2 emitted by US road transport at a resolution of 1 km annually for 1980-2012. DARTE reveals that urban areas are responsible for 80% of on-road emissions growth since 1980 and for 63% of total 2012 emissions. We observe nonlinearities between CO 2 emissions and population density at broad spatial/temporal scales, with total on-road CO 2 increasing nonlinearly with population density, rapidly up to 1,650 persons per square kilometer and slowly thereafter. Per capita emissions decline as density rises, but at markedly varying rates depending on existing densities. We make use of DARTE's bottom-up construction to highlight the biases associated with the common practice of using population as a linear proxy for disaggregating national-or state-scale emissions. Comparing DARTE with existing downscaled inventories, we find biases of 100% or more in the spatial distribution of urban and rural emissions, largely driven by mismatches between inventory downscaling proxies and the actual spatial patterns of vehicle activity at urban scales. Given cities' dual importance as sources of CO 2 and an emerging nexus of climate mitigation initiatives, high-resolution estimates such as DARTE are critical both for accurately quantifying surface carbon fluxes and for verifying the effectiveness of emissions mitigation efforts at urban scales.emissions | carbon dioxide | urban | transportation | on-road