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High-resolution albedo has the advantage of a higher spatial scale from tens to hundreds of meters, which can fill the gaps of albedo applications from the global scale to the regional scale and can solve problems related to land use change and ecosystems. The Sentinel-2 satellite provides high-resolution observations in the visible-to-NIR bands, giving possibilities to generate a high-resolution surface albedo at 10 m. This study attempted to evaluate the performance of the four data-driven machine learning algorithms (i.e., random forest (RF), artificial neural network (ANN), k-nearest neighbor (KNN), and XGBoost (XGBT)) for the generation of a Sentinel-2 albedo over flat and rugged terrain. First, we used the RossThick-LiSparseR model and the 3D discrete anisotropic radiative transfer (DART) model to build the narrowband surface reflectance and broadband surface albedo, which acted as the training and testing datasets over flat and rugged terrain. Second, we used the training and testing datasets to drive the four machine learning models, and evaluated the performance of these machine learning models for the generation of Sentinel-2 albedo. Finally, we used the four machine learning models to generate a Sentinel-2 albedo and compared them with in situ albedos to show the models’ application potentials. The results show that these machine learning models have great performance in estimating Sentinel-2 albedos at a 10 m spatial scale. The comparison with in situ albedos shows that the random forest model outperformed the others in estimating a high-resolution surface albedo based on Sentinel-2 datasets over the flat and rugged terrain, with an RMSE smaller than 0.0308 and R2 larger than 0.9472.