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High-Curie-temperature (Tc) 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 Tc 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 photoferroel