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Organic Dye Passivation for High‐Performance All‐Inorganic CsPbI1.5Br1.5 Perovskite Solar Cells with Efficiency over 14%

All‐inorganic perovskite solar cells (PSCs) have recently received growing attention as a promising template to solve the thermal instability of organic–inorganic PSCs. However, the thermodynamic phase instability and relatively low device efficiency pose challenges. Herein, highly efficient and stable CsPbI1.5Br1.5 compositional perovskite‐based inorganic PSCs are fabricated using an organic dye, fluorescein isothiocyanate (FITC), as a passivator. The carboxyl and thiocyanate groups of FITC not only minimize the trap states by forming interactions with the under‐coordinated Pb2+ ions but also significantly increase the grain size and improve the crystallinity of the perovskite films during annealing. Consequently, perovskite films with superior optoelectronic properties, prolonged carrier lifetime, reduced trap density, and improved stability are obtained. The resulting device yields a champion efficiency of 14.05% with negligible hysteresis, which presents the highest reported efficiency for inorganic CsPbI1.5Br1.5 solar cells reported thus far. In addition, FITC can be generally adopted as attractive passivator to improve the performance of CsPbI2Br‐ and CsPbIBr2‐based PSCs. Furthermore, with a comprehensive comparison of mixed‐halide inorganic perovskites, it is demonstrated that CsPbI1.5Br1.5 compositional perovskite is a promising candidate with the optimal halide composition for high‐performance inorganic PSCs.