We employed an optimal interpolation (OI) method to assimilate AIRNow ozone/PM2.5 and MODIS (Moderate Resolution Imaging Spectroradiometer) aerosol optical depth (AOD) data into the Community Multi-scale Air Quality (CMAQ) model to improve the ozone and total aerosol concentration for the CMAQ simulation over the contiguous United States (CONUS). AIRNow data assimilation was applied to the boundary layer, and MODIS AOD data were used to adjust total column aerosol. Four OI cases were designed to examine the effects of uncertainty setting and assimilation time; two of these cases used uncertainties that varied in time and location, or "dynamic uncertainties." More frequent assimilation and higher model uncertainties pushed the modeled results closer to the observation. Our comparison over a 24-hr period showed that ozone and PM 2.5 mean biases could be reduced from 2.54 ppbV to 1.06 ppbV and from -7.14 µg/m 3 to -0.11 µg/m 3 , respectively, over CONUS, while their correlations were also improved. Comparison to DISCOVER-AQ 2011 aircraft measurement showed that surface ozone assimilation applied to the CMAQ simulation improves regional low-altitude (below 2 km) ozone simulation. Implications: This paper described an application of using optimal interpolation method to improve the model's ozone and PM 2.5 estimation using surface measurement and satellite AOD. It highlights the usage of the operational AIRNow data set, which is available in near real time, and the MODIS AOD. With a similar method, we can also use other satellite products, such as the latest VIIRS products, to improve PM 2.5 prediction.