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This paper describes the third part of a series of investigations to develop algorithms for simultaneous retrieval of aerosol parameters and surface spectral reflectance from GEOstationary Trace gas and Aerosol Sensor Optimization (GEO-TASO) instrument. Since the algorithm is designed for future hyperspectral and geostationary satellite sensors, such as Tropospheric Emissions: Monitoring of Pollution (TEMPO), it is applied to GEO-TASO data measured over the same area by different flights as part of the Korea-United Stated Air Quality Study (KORUS-AQ) field campaign in 2016. While GEO-TASO has a spectral sampling interval of ~0.28 nm in the visible, its data is thinned through a band selection approach with consideration of atmospheric transmittance and different surface types, which yields 20 common spectral bands to be used by the algorithm. The algorithm starts with 4 common principal components (PCs) for surface spectral reflectance extracted from various spectral libraries; constraints of surface reflectance and aerosol model parameters are obtained respectively from k-means clustering analysis of the Rayleighcorrected GEO-TASO spectra and AERONET data. The algorithm then proceeds iteratively with an optimal estimation approach to update PCs and retrieve aerosol optical depth (AOD) from GEO-TASO measured spectra until state vector converges. The comparison of AODs between GEO-TASO retrievals (y) and 7 AERONET (x) sites reveals that the iterative updates of surface PCs (and so surface reflectance) improve the inversions of fine-mode AOD, fine-mode fraction of AOD, Ångström exponent, and AOD at all (440, 550, 550, 675 nm) wavelengths. At 440 nm, the linear fitting equation, the Pearson correlation coefficient (R2 ), and mean absolute error are improved respectively from y = 0.72x + 0.11, 0.53, and 0.05 (without update of PCs) to y = 1.055x + 0.01, 0.76, and 0.033. Future work is to prepare the algorithm for TEMPO that carries an enhanced version of GEO-TASO instrument.