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Tin dioxide (SnO2), one of the best electron transport layer materials for perovskite solar cells (PSCs), has high electrical conductivity and low photocatalytic activity. However, the defects in its inside and surface result in nonradiative recombination at the SnO2/perovskite interface. Complex and time‐consuming passivation methods are not conducive to the commercialization of PSCs, and simple passivation strategies should be used to improve the photovoltaic performance of the devices. Herein, a facile and efficient method is proposed to simultaneously passivate the inside and surface defects by adding histidine (HIS) to SnO2 colloidal solution. This one‐step doping strategy also modulates carrier dynamics at the SnO2/perovskite interface. HIS reduces suspended hydroxyl groups, oxygen vacancies, and uncoordinated Sn4+ defects on the surface of SnO2, as well as uncoordinated Pb2+ and halogen vacancy defects at the buried interface of perovskite. Surprisingly, HIS can prevent perovskite from decomposition to form PbI2, which further decomposes to photoactive metallic Pb0 and I, causing ion migration in PSC. As a result, the PSC efficiency has significantly improved 23.11% after HIS doping. The efficiency of unencapsulated device with HIS is 94% of the primary efficiency after storage in relative humidity = 70 ± 5% for 1000 h. [ABSTRACT FROM AUTHOR]