Ferroelectrics, as piezoelectric materials with reversal polarization, have great appeal in energy signal harvesting and conversion. Their polarization and piezoelectricity are widely used in various smart devices such as data storage, sensors, solar cells, and self-powered systems. Among them, multiaxial molecular ferroelectrics with multiple equivalent polarization directions are highly preferred for such applications. However, designing and regulating multiaxial molecular ferroelectrics has always been a huge challenge, especially in those with excellent piezoelectric performance. Here, under precise molecular modifications, we successfully designed and regulated four high-temperature multiaxial molecular ferroelectrics, [(CH₃)₃NCH₂X]FeBr₄ (X = F, Cl, Br, I). More strikingly, piezoresponse force microscopy demonstrates that [(CH₃)₃NCH₂F]FeBr₄ exhibits a relatively large piezoelectric response comparable with that of polyvinylidene fluoride. This precise molecular design strategy provides an effective means for the acquisition and regulation of multiaxial molecular ferroelectrics, offering new opportunities for modern energy and artificial intelligence.

铁电体，作为具有反向极化的压电材料，在能量信号采集和转换中具有巨大的吸引力。它们的极化和压电特性广泛用于各种智能设备，例如数据存储，传感器，太阳能电池和自供电系统。在这些应用中，具有多个等效极化方向的多轴分子铁电体是高度优选的。然而，设计和调节多轴分子铁电体一直是一个巨大的挑战，特别是在压电性能优异的情况下。在这里，通过精确的分子修饰，我们成功设计并调节了四种高温多轴分子铁电体，[（CH ₃）₃ NCH ₂ X] FeBr ₄（X ＝ F，Cl，Br，I）。更加显着的是，压电响应力显微镜显示[（CH ₃）₃ NCH ₂ F] FeBr ₄表现出与聚偏二氟乙烯相当的压电响应。这种精确的分子设计策略为获取和调节多轴分子铁电体提供了有效的手段，为现代能源和人工智能提供了新的机会。