Gas and aerosol predictions from CMAQ simulations with horizontal grid spacings of 8- and 32-km are evaluated against available observations from CASTNet, IMPROVE, AIRS-AQS, SOS99/SOS99NASH, SEARCH, and ARIES for the southeastern US for the period of 1–10 July 1999. The predictions evaluated in this work include mixing ratios of O 3 (hourly, maximum 1-h, and 8-h average), NO x , HNO 3, NO y , and mass concentrations of PM 10, PM 2.5, and PM 2.5 components. Our evaluation has shown that CMAQ tends to underpredict maximum 1-h O 3 mixing ratios on high O 3 days at some sites. It overpredicts the maximum and minimum hourly O 3 mixing ratios for most low O 3 days, the daytime and nighttime hourly, and the maximum 8-h average O 3 mixing ratios on most days at all sites. The model performance for hourly O 3 mixing ratios generally meets EPA's criteria but deteriorates for maximum 1- and 8-h average O 3 mixing ratios. CMAQ underpredicts the mass concentrations of PM 10, PM 2.5, and PM 2.5 composition and fails to reproduce their temporal variations (except for sulfate). Largest underpredictions occur for organic matter (OM 2.5) and nitrate 2.5 among all PM components. These underpredictions and overpredictions may be caused by inaccurate meteorological predictions (e.g., the PBL height, wind speed/direction, vertical mixing, temperature, and relative humidity) and boundary conditions for chemical species (e.g., O 3), underestimation in emissions (e.g., NO x , NH 3, and primary OM), as well as uncertainties in model assumptions and treatments in aerosol chemistry and microphysics.