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Inorganic semiconductor ferroelectrics such as BiFeO₃ have shown great potential in photovoltaic and other applications. Currently, semiconducting properties and the corresponding application in optoelectronic devices of hybrid organo-plumbate or stannate are a hot topic of academic research; more and more of such hybrids have been synthesized. Structurally, these hybrids are suitable for exploration of ferroelectricity. Therefore, the design of molecular ferroelectric semiconductors based on these hybrids provides a possibility to obtain new or high-performance semiconductor ferroelectrics. Here we investigated Pb-layered perovskites, and found the layer perovskite (benzylammonium)₂PbCl₄ is ferroelectric with semiconducting behaviours. It has a larger ferroelectric spontaneous polarization P_s=13 μC cm⁻² and a higher Curie temperature T_c=438 K with a band gap of 3.65 eV. This finding throws light on …