Tailoring well-defined interfacial structures of heterogeneous metal catalysts has become an effective strategy for identifying the interface relationships and facilitating the reactions involving multiple intermediates. Here, a particle-particle heterostructure catalyst consisting of Pd and copper oxide nanoparticles is designed to achieve high-performance alkaline methanol oxidation electrocatalysis. The strong coupling particle-particle heterostructure catalyst induced a unique interfacial interpenetration effect to improve the interfacial charge redistribution and regulate the