AbstractInorganic perovskite solar cells (IPSCs) have developed rapidly due to their good thermal stability and the bandgap suitable for perovskite/silicon tandem solar cells. However, the large open‐circuit voltage (VOC) deficit derived from the surface defects and the energy level structure mismatch impede the development of device performance, especially in the P‐I‐N structure IPSCs. Herein, an innovative in situ etching (ISE) treatment method is proposed to reduce surface defects through methanol without additional passivator. It is found that the perovskite films treated with methanol result in a slight excess of PbI2 on the surface and inserted into the grain boundaries. Therefore, the successful decrease of surface defects by methanol and the passivation of grain boundary defects by PbI2 greatly reduce the trap density of perovskite films. And the larger work function of PbI2 contributes to the energy band of perovskite surface bending downward and forms gradient energy level alignment at the I/N interface, which accelerates extraction of charge carriers. As a result, the efficiency of CsPbI2.85Br0.15 inverted IPSC is enhanced from 16.00% to 19.34%, which is one of the mostly efficient IPSCs. This work provides an original idea without additional passivator to manage the defects of inorganic perovskite.