Performance Enhancement of All‐Inorganic CsPbI 3 Perovskite Solar Cells through Functional Additive and Buried Interface Engineering

All‐inorganic CsPbI 3 perovskite solar cells (IPSCs) are regarded as promising candidates due to their ideal bandgap and excellent thermal stability. However, their practical application is hindered by phase instability and severe interfacial defects, which lead to performance degradation and poor durability. Here, this work proposes a low‐temperature synergistic regulation strategy that combines oxamide additive with potassium tartrate interfacial modification to simultaneously optimize interface and adjust bulk crystallization process of CsPbI 3 film. The incorporation of oxamide effectively suppresses iodide vacancy defects, promotes uniform crystal growth and reduces non‐radiative recombination, while the buried‐interface modification by potassium tartrate regulates the energy‐level alignment, passivates interfacial traps and promotes carrier extraction. Benefiting from this dual regulation, the modified CsPbI 3 ‐based IPSCs achieve a power conversion efficiency of 18.89% and exhibit significantly improved environmental stability. This work provides a simple, effective and scalable approach to address the intrinsic phase instability and interfacial defect problems in CsPbI 3 ‐based IPSCs.