AbstractThe rational design for transition metals‐based carbon nano‐materials as efficient electrocatalysts still remains a crucial challenge for economical electrochemical hydrogen production. Carbon nanotubes (CNTs) as attractive electrocatalysts are typically activated by non‐metal dopant to promote catalytic performance. Metals doping or metal/non‐metal co‐doping of CNTs, however, are rarely explored. Herein, this work rationally designs bimetal oxide templates of ZnCo₂O₄ for heterogeneously doping Zn and N into Co nanoparticles embedded carbon nanotubes (Co@Zn‐N‐CNTs). During the formation of CNTs, Zn atoms volatilize from ZnCo₂O₄ and in situ dope into the carbon skeleton. In particular, owing to the low electronegativity of Zn, the electrons aptly transfer from Zn to carbon atoms, which generate a high electron density for the carbon layers and offer more preponderant catalytic sites for hydrogen reduction. The Co@Zn‐N‐CNTs catalyst exhibits enhanced hydrogen evolution reaction activity in 0.5 m H₂SO₄ electrolyte, with a low onset potential of −20 mV versus RHE at 1 mA cm⁻², an overpotential of 67 mV at 10 mA cm⁻², a small Tafel slope of 52.1 mV dec⁻¹, and persistent long‐term stability. This study provides brand‐new insights into the utilization of Zn as electronic regulator and activity promoter toward the design of high‐efficiency electrocatalysts.