We present a new calibration method to derive aerosol optical depth (AOD) from the MultiFilter Rotating Shadowband Radiometer (MFRSR) under extremely hazy atmospheric conditions during the East Asian Study of Tropospheric Aerosols: an International Regional Experiment (EAST-AIRE) and the Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) deployment in China. MFRSR measurements have been made at Xianghe since September 2004 and at Taihu and Shouxian since March and May 2008, respectively. Aerosol property retrievals from CIMEL Electonique, Paris, Sun and sky radiometers located at each site show that aerosol loading is substantial and highly variable during a given year (averaged daily AOD550 = 0.80 ± 0.14). The conventional application of the Langley method to calibrate the MFRSR is not possible at these sites because there is a dearth of stable atmospheric and low-AOD conditions. To overcome this limitation of the traditional Langley plot method, highest irradiance values at a given air mass during a given period are used here. These highest values can represent the clear-sky and minimum aerosol loading conditions. A scatterplot of the AOD estimated by this method with the CIMEL Sun and sky radiometer AOD shows very good agreement: correlation coefficients are on the order of 0.98–0.99, slopes range from 0.93 to 0.97, and offsets are less than 0.02 for the three sites. AOD and Ångström exponents were derived from application of the method to all MFRSR data acquired at the three sites. AOD values at 500 nm are τ500 = 0.99 ± 0.71 (α500–870 = 1.45 ± 0.59) at Xianghe, 0.87 ± 0.54 (1.14 ± 0.31) at Taihu, and 0.84 ± 0.43 (1.15 ± 0.28) at Shouxian. Anthropogenic aerosols appear to dominate in the study region with significant contributions from large dust particles and influence of hydroscopic growth.