Fabricating poly(vinylidene fluoride) (PVDF) and its composite ferroelectrics are essential for the development of next-generation lightweight, portable, wearable, and implantable intelligent devices. However, integrating and maximizing spontaneous polarization and interfacial electromechanical conversion efficiency remain major challenges in the contemporary PVDF-based composites field. Herein, inspired by the tenon-and-mortise structure associated with ancient Chinese architecture, an amino-anchored metal-organic framework (MOF)/PVDF piezoelectric composite using a dipole-engineering strategy to deliver enhanced piezocatalytic performance is constructed. Homogeneous and long-range ordered hydrogen-bond networks have been formed with the PVDF matrix after introducing periodically arranged amino anchors into the NH