Structural defects are ubiquitous for polycrystalline perovskite films, compromising device performance and stability. Herein, a universal method is developed to overcome this issue by incorporating halide perovskite quantum dots (QDs) into perovskite polycrystalline films. CsPbBr3 QDs are deposited on four types of halide perovskite films (CsPbBr3, CsPbIBr2, CsPbBrI2, and MAPbI3) and the interactions are triggered by annealing. The ions in the CsPbBr3 QDs are released into the thin films to passivate defects, and concurrently the hydrophobic ligands of QDs self‐assemble on the film surfaces and grain boundaries to reduce the defect density and enhance the film stability. For all QD‐treated films, PL emission intensity and carrier lifetime are significantly improved, and surface morphology and composition uniformity are also optimized. Furthermore, after the QD treatment, light‐induced phase segregation and degradation in mixed‐halide perovskite films are suppressed, and the efficiency of mixed‐halide CsPbIBr2 solar cells is remarkably improved to over 11% from 8.7%. Overall, this work provides a general approach to achieving high‐quality halide perovskite films with suppressed phase segregation, reduced defects, and enhanced stability for optoelectronic applications.
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