The Soil Moisture Ocean Salinity (SMOS) was the first mission providing L-band multi-angular brightness temperature (TB) at the global scale. However, radio frequency interferences (RFI) and aliasing effects degrade, when present SMOS TBs, and thus affect the retrieval of land parameters. To alleviate this, a refined SMOS multi-angular TB dataset was generated based on a two-step regression approach. This approach smooths the TBs and reconstructs data at the incidence angle with large TB uncertainties. Compared with Centre Aval de Traitement des Données SMOS (CATDS) TB product, this dataset shows a better relationship with the Soil Moisture Active Passive (SMAP) TB and enhanced correlation with in-situ measured soil moisture. This RFI-suppressed SMOS TB dataset, spanning more than a decade (since 2010), is expected to provide opportunities for better retrieval of land parameters and scientific applications.