In the U.S., emissions of greenhouse gases and air pollutants are often developed independently. Here, we describe the GReenhouse gas And Air Pollutants Emissions System (GRA2PES), which provides gridded emissions of fossil-fuel carbon dioxide (ffCO2) and 93 air quality (AQ) species for 17 combustion and non-combustion sectors at 4 km × 4 km spatial resolution across the contiguous US. We find that the AQ emissions most spatially correlated with ffCO2 are nitrogen oxides (NOx, ρ = 0.67), followed by sulfur dioxide (SO2, ρ = 0.51), carbon monoxide (CO, ρ = 0.44), and fine particulate matter (PM2.5, ρ = 0.38). We evaluate GRA2PES ffCO2 emissions with an ensemble of publicly available regional and global inventories at national (Normalized Mean Bias (NMB) = +1.4\%), state (NMB = +1.5\%, R2 = 0.98), and urban (NMB = +11.5\%, R2 = 0.97) scales. Nationally, the differences of publicly available inventories from the ensemble average range from −10.0\% to +5.7\%, and consistency diverges at state and urban scales. We simulate GRA2PES ffCO2 in a particle dispersion model and compare to measurements of radiocarbon (14C)-derived ffCO2 collected in Los Angeles (August 2021), with results suggesting that GRA2PES ffCO2 may be low by 19\% for this city, but well within model-observation differences for other publicly available inventories (−43\% to +94\%). GRA2PES AQ/ffCO2 ratios converted to concentration space generally agree with field observations (NMB = +4\%, log R2 = 0.90). Lastly, we present a method by which to utilize GRA2PES to derive AQ emission fluxes from ffCO2 emissions.