摘要: Multiferroic materials that combine ferroelectricity and ferroelasticity can exhibit switchable spontaneous polarization/strain responses, bringing potential applications in new intelligent actuators, sensors and memory devices. However, due to the strict requirements for polar crystal symmetry and specific structural phase transitions, organic-inorganic halide multiferroics remain very rare, with zinc-based ones constituting a blank. Here, by implementing halogen engineering, we successfully designed and synthesized a zinc-based hybrid multiferroic material (CTA)2ZnI4 (CTA = cyanomethyltriethylammonium), which undergoes a mm2Fm-type ferroic phase transition at Curie temperature of 404 K. The halogen substitution strategy on ZnX4 tetrahedra effectively regulates the weak molecular interactions between organic and inorganic components, not only significantly increasing the Curie temperature by 55 K, but also successfully inducing ferroelectric and ferroelastic properties. To our knowledge, (CTA)2ZnI4 is the first case of zinc-based organic-inorganic halide multiferroics to date. This work provides a valuable reference for designing hybrid multiferroics towards multi-modal information processing applications.