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Aerosols in the atmosphere play an essential role in the radiative transfer process due to their scattering, absorption, and emission. Moreover, they interrupt the retrieval of atmospheric properties from ground-based and satellite remote sensing. Thus, accurate aerosol information needs to be obtained. Herein, we developed an optimal-estimation-based aerosol optical depth (AOD) retrieval algorithm using the hyperspectral infrared downwelling emitted radiance of the Atmospheric Emitted Radiance Interferometer (AERI). The proposed algorithm is based on the phenomena that the thermal infrared radiance measured by a ground-based remote sensor is sensitive to the thermodynamic profile and degree of the turbid aerosol in the atmosphere. To assess the performance of algorithm, AERI observations, measured throughout the day on 21 October 2010 at Anmyeon, South Korea, were used. The derived thermodynamic profiles and AODs were compared with those of the European center for a reanalysis of medium-range weather forecasts version 5 and global atmosphere watch precision-filter radiometer (GAW-PFR), respectively. The radiances simulated with aerosol information were more suitable for the AERI-observed radiance than those without aerosol (i.e., clear sky). The temporal variation trend of the retrieved AOD matched that of GAW-PFR well, although small discrepancies were present at high aerosol concentrations. This provides a potential possibility for the retrieval of nighttime AOD.