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High-Curie-temperature (T_c) ferroelectrics have exhibited broad applications in optoelectronic devices. Recently, two-dimensional multilayered perovskite ferroelectrics with excellent photoelectric attributes are attracting increasing interest as new systems of photoferroelectrics. However, the effective tuning of the T_c value of a multilayered perovskite photoferroelectric system still remains a huge challenge. Here, by a halogen substitution strategy to introduce bromine atoms on n-propylamine cations, the hybrid perovskite photoferroelectric (3-bromopropylaminium)₂(formamidinium)Pb₂Br₇ (BFPB) with a high T_c value (348.5 K) was obtained. It is notable that BFPB adopts a two-dimensional bilayered inorganic framework, with tight linking to the organic cation by C–Br···Br–Pb halogen···halogen interactions and N–H···Br hydrogen bonds. Intriguingly, in comparison with the prototypical compound (n-propylaminium)₂ …