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In recent years, developing dopant‐free carrier‐selective contacts, instead of heavily doped Si layer (either externally or internally), for crystalline silicon (c‐Si) solar cells have attracted considerable interests with the aim to reduce parasitic light absorption and fabrication cost. However, the stability still remains a big challenge for dopant‐free contacts, especially when thermal treatment is involved, which limits their industrial adoption. In this study, a perovskite material ZnTiO3 combining with an ultrathin (~1 nm) SiO2 film and Al layer is used as an electron‐selective contact, forming an isotype heterojunction with n‐type c‐Si. The perovskite/c‐Si heterojunction solar cells exhibit a performance‐enhanced effect by postmetallization annealing when the annealing temperature is 200–350°C. Thanks to the postannealing treatment, an impressive efficiency of 22.0% has been demonstrated, which is 3.5% in absolute value higher than that of the as‐fabricated solar cell. A detailed material and device characterization reveal that postannealing leads to the diffusion of Al into ZnTiO3 film, thus doping the film and reducing its work function. Besides, the coverage of SiO2 is also improved. Both these two factors contribute to the enhanced passivation effect and electron selectivity of the ZnTiO3‐based contact and hence improve the cell performance. [ABSTRACT FROM AUTHOR]