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Interface engineering is deemed as an effective approach to optimize the electronic structure of catalytically active sites in electrocatalysts for boosted hydrogen evolution reaction (HER). Herein, a novel ultrasmall VN/Co heterostructure anchored in N-doped graphitized nanocarbons (VN/Co@GNC) is successfully synthesized by a simple calcination protocol. Benefiting from the abundant reactive sites on the interface of ultrasmall heterostructure, enhanced N active sites of VN coupled with Co nanoparticles, as well as excellent conductivity of N-doped graphitized nanocarbons as the scaffold, the resulting VN/Co@GNC material exhibits outstanding electrocatalytic HER performance, delivering the current density of 10 mA/cm2 at a quite low overpotential of 155 mV without iR-compensation, and retaining the catalytic durability for at least 565 h (∼23.5 days) in 1 M KOH solution. The superior catalytic activity and ultrastability of VN/Co@GNC electrocatalyst lay a solid foundation for its commercial applications toward the hydrogen fuel production.