Piezocatalysis in aqueous medium has shown great potential for various applications, however the efficiency of piezocatalytic nanoparticles is harmed by the limited utilization of piezoelectric charge and the lack of active catalytic interface. In this study, BaTiO3@Metal (BTO@M, M=Pt, Pd and Au) hetero‐nanostructures were synthesized by using a piezodeposition method. The deposited metal cocatalysts significantly promote the separation and migration of piezogenerated charge, consequently enhancing the piezocatalytic reactions on different metal cocatalyst interfaces. Specifically, BTO@Au under ultrasonic vibrations exhibited most efficient generation of reactive oxidative species via a two‐electron reduction pathway in the presence of dissolved oxygen, while BTO@Pt showed promoted hydrogen evolution in the absence of oxygen. The metal‐piezoelectric hetero‐nanostructures proposed in this work highlight the key role of noble metal as cocatalysts for piezoelectricity‐driven oxygen reduction and hydrogen evolution reactions, which could further advance piezocatalysis in the field of clean energy, water disinfection and biomedicine.