Aerosol single scattering albedo (SSA) can be retrieved from the ratio of diffuse horizontal and direct normal fluxes measured from multifilter rotating shadowband radiometer (MFRSR). In this study, the measurement channels at 415nm and 870nm are selected for aerosol optical depth (AOD) and Angstrom coefficient retrievals, and the measurements at 415nm are used for aerosol SSA retrievals with the constraint of retrieved Angstrom coefficient. We extensively assessed various issues impacting on the accuracy of SSA retrieval from measurements to input parameters and assumptions. For cloud-free days with mean aerosol loading of 0.13–0.60, our sensitivity study indicated that: (1) 1% calibration uncertainty can result in 0.8–3.7% changes in retrieved SSA; (2) without considering the cosine respond correction and/or forward scattering correction will result in underestimation of 1.1–3.3% and/or 0.73% in retrieved SSA; (3) an overestimation of 0.1 in asymmetry factor can result in an underestimation of 2.54–3.4% in retrieved SSA; (4) for small aerosol loading (e.g., 0.13), the uncertainty associated with the choice of Rayleigh optical depth value can result in non-negligible change in retrieved SSA (e.g., 0.015); (5) an uncertainty of 0.05 for surface albedo can result in changes of 1.49–5.4% in retrieved SSA. We applied the retrieval algorithm to the MFRSR measurements at the Atmospheric Radiation Measurements (ARM) Southern Great Plains (SGP) site. The retrieved results of AOD, Angstrom coefficient, and SSA are basically consistent with other independent measurements from co-located instruments at the site.