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Abstract Designing high efficiency platinum (Pt)‐based catalysts for methanol oxidation reaction (MOR) with high “non‐CO” pathway selectivity is strongly desired and remains a grand challenge. Herein, PtRuNiCoFeGaPbW HEA ultrathin nanowires (HEA‐8 UNWs) are synthesized, featuring unique cascaded p–d orbital hybridization interaction by inducing dual p‐block metals (Ga and Pb). In comparison with Pt/C, HEA‐8 UNWs exhibit 15.0‐ and 4.2‐times promotion of specific and mass activity for MOR. More importantly, electrochemical in situ FITR spectroscopy reveals that the production/adsorption of CO (CO*) intermediate is effectively avoided on HEA‐8 UNWs, leading to the complete “non‐CO” pathway for MOR. Theoretical calculations demonstrate the optimized electronic structure of HEA‐8 UNWs can facilitates a lower energy barrier for the “non‐CO” pathway in the MOR.