There is a pressing need to verify air pollutant and greenhouse gas emissions from anthropogenic fossil energy sources to enforce current and future regulations. We demonstrate the feasibility of using simultaneous remote sensing observations of column abundances of CO₂, CO, and NO₂ to inform and verify emission inventories. We report, to our knowledge, the first ever simultaneous column enhancements in CO₂ (3–10 ppm) and NO₂ (1–3 Dobson Units), and evidence of δ¹³CO₂ depletion in an urban region with two large coal-fired power plants with distinct scrubbing technologies that have resulted in ∆NO_x/∆CO₂ emission ratios that differ by a factor of two. Ground-based total atmospheric column trace gas abundances change synchronously and correlate well with simultaneous in situ point measurements during plume interceptions. Emission ratios of ∆NO_x/∆CO₂ and ∆SO₂/∆CO₂ derived from in situ atmospheric observations agree with those reported by in-stack monitors. Forward simulations using in-stack emissions agree with remote column CO₂ and NO₂ plume observations after fine scale adjustments. Both observed and simulated column ∆NO₂/∆CO₂ ratios indicate that a large fraction (70–75%) of the region is polluted. We demonstrate that the column emission ratios of ∆NO₂/∆CO₂ can resolve changes from day-to-day variation in sources with distinct emission factors (clean and dirty power plants, urban, and fires). We apportion these sources by using NO₂, SO₂, and CO as signatures. Our high-frequency remote sensing observations of CO₂ and coemitted pollutants offer promise for the verification of power plant emission factors and abatement technologies from ground and space.