The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/admi.202200179. solar cells. [2] Recently, perovskite solar cells (PSCs) have gained enormous attention owing to their tunable energy bandgap, long charge carrier diffusion length, and high absorption coefficient. [3] The photoelectric conversion efficiency (PCE) of PSCs has increased rapidly from 3.8% to 25.5% certified by the National Renewable Energy Laboratory of the United States. [4] Its rapid progress has never been seen before in the history of photovoltaic development. However, many obstacles should be overcome for its large-scale commercialization, such as the currentvoltage hysteresis effect, long-term instability (lifetime), and degradation under oxygen-rich or humidity. [5] In the preparation process of the perovskite layer, many point defects will appear such as vacancies, interstitial, or anti-site atoms (MAPbI 3 , e.