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We explore a synergistic approach to use the complementary angular samplings from the Multi-angle Imaging SpectroRadiometer (MISR) and Moderate Resolution Imaging Spectroradiometer (MODIS) to improve MODIS surface bidirectional reflectance distribution function (BRDF) and albedo retrieval. Preliminary case studies show that MODIS and MISR surface bidirectional reflectance factors (BRFs) are generally comparable in the green, red, and near infrared. An information index is introduced to characterize the information content of directional samplings, and it is found that MISR angular observations can bring additional information to the MODIS retrieval, especially when the MISR observations are close to the principal plane. We use the BRDF parameters derived from the MISR surface BRFs as a priori information and derive a posteriori estimates of surface BRDF parameters with the MODIS observations. Results show that adding MISR angular samplings can reduce the relative BRF prediction error by up to 10% in the red and green, compared to the retrievals from MODIS-only observations which are close to the cross-principal plane.