A Comprehensive Air-Quality Model with Extensions (CAMx) version 6.10 simulation was assessed through comparison with data acquired during NASA’s 2011 Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Maryland field campaign. Comparisons for the baseline simulation (Carbon Bond 2005 (CB05) chemistry, Environmental Protection Agency 2011 National Emissions Inventory) show a model overestimate of NOy by +86.2% and an underestimate of HCHO by 28.3%. We present a new model framework (Carbon Bond 6 Revision 2 chemistry (CB6r2), Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.1 biogenic emissions, 50% reduction in mobile NOx, enhanced representation of isoprene nitrates) that better matches observations. The new model framework attributes 31.4% more surface ozone in Maryland to electric generating units (EGUs) and 34.6% less ozone to on-road mobile sources. Surface ozone becomes more NOx limited throughout the eastern United States compared to the baseline simulation. The baseline model therefore likely underestimates the effectiveness of anthropogenic NOx reductions as well as the current contribution of EGUs to surface ozone.