Strong metal‐support interaction (SMSI) is crucial for supported catalysts in heterogeneous catalysis. Here is the first report on strong metal phosphide‐phosphate support interaction (SMPSI). The key to SMPSI is the activation of P species on the support, which leads to simultaneous generation of metal phosphide nanoparticles (NPs) and core–shell nanostructures formed by support migration onto the NPs. The encapsulation state of metal phosphide and charge transfer are identical to those of classical SMSIs and can be optimally regulated. Furthermore, the strong interactions of Co2PL/MnP‐3 not only significantly enhance the anti‐oxidation and anti‐acid capability of non‐noble metal but also exhibit excellent catalytic activity and stability toward hydrogenating a wide range of compounds into value‐added fine chemicals with 100% selectivity, which is even better than Pd/C and Pt/C. The SMPSI construction can be generally extended to other systems such as Ni2PL/Mn3(PO4)2, Co2PL/LaPO4, and CoPL/CePO4. This study provides a new approach for the rational design of advanced non‐noble metal catalysts and introduce a novel paradigm for the strong interaction between NPs and support.

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