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The prominent chemical bath deposition (CBD) method leverages tin dioxide (SnO2) as an electron transport layer (ETL) in perovskite solar cells (PSCs), achieving exceptional efficiency. The deposition of SnO2, however, can lead to the formation of oxygen vacancies and surface defects, which subsequently contribute to performance challenges such as hysteresis and instability under light‐soaking conditions. To alleviate these issues, it is crucial to address heterointerface defects and ensure the uniform coverage of SnO2 on fluorine‐doped tin oxide substrates. Herein, the efficacy of tin(IV) chloride (SnCl4) post‐treatment in enhancing the properties of the SnO2‐ETL and the performances of PSCs are presented. The treatment with SnCl4 not only removes undesired agglomerated SnO2 nanoparticles from the surface of CBD SnO2 but also improves its crystallinity through a recrystallization process. This leads to an optimized interface between the SnO2‐ETL and perovskite, effectively minimizing defects while promoting efficient electron transport. The resultant PSCs demonstrate improved performance, achieving an efficiency of 25.56% (certified with 24.92%), while retaining 95.84% of the initial PCE under ambient storage conditions. Additionally, PSCs treated with SnCl4 endure prolonged light‐soaking tests, particularly when subjected to quasi‐steady‐state‐IV measurements. This highlights the potential of SnCl4 treatment as a promising strategy for advancing PSC technology. [ABSTRACT FROM AUTHOR]