Retrieval of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) using the Collection 5 (C005) algorithm provides large-scale (10 × 10 km) estimates that can be used to predict surface layer concentrations of particulate matter with aerodynamic diameter smaller than 2.5 µm (PM2.5). However, these large-scale estimates are not suitable for identifying intraurban variability of surface PM2.5 concentrations during wildfire events when individual plumes impact populated areas. We demonstrate a method for providing high-resolution (2.5 km) kernel-smoothed estimates of AOD over California during the 2008 northern California fires. The method uses high-resolution surface reflectance ratios of the 0.66 and 2.12 µm channels, a locally derived aerosol optical model characteristic of fresh wildfire plumes, and a relaxed cloud filter. Results show that the AOD derived for the 2008 northern California fires outperformed the standard product in matching observed aerosol optical thickness at three coastal Aerosol Robotic Network sites and routinely explained more than 50% of the variance in hourly surface PM2.5 concentrations observed during the wildfires.