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Designing high-performance, cost-effective, and durable electrocatalysts for hydrogen evolution reactions is essential and challenging. The design of electrode surface architecture to accomplish rapid gas bubble release is a promising strategy. Herein, we design a unique network-structured catalyst by constructing NiFe alloy on a submicron carbon fiber network substrate (NiFe/SCFN). The unique structure imparts superaerophobicity to NiFe/SCFN and facilitates gas bubbles removal, thereby accelerating mass transfer. Benefiting from electrode alloying, the hydrogen adsorption free energy was reduced to − 0.026 eV (Fe sites) and 0.077 eV (Ni sites) on the catalyst surface, improving the electronic conductivity. NiFe/SCFN achieves low overpotentials of 19.2 mV and 199 mV at 10 mA∙cm−2 and 100 mA∙cm−2 with excellent stability, owing to the unique network structure and the NiFe alloy's electronic structure. This work provides a new strategy for designing effective catalysts with transition metals. [Display omitted] • The unique network structure endows the catalyst superaerophobic characteristics. • The hydrogen adsorption free energy is reduced to ‐0.026 eV (Fe sites) and 0.077 eV (Ni sites). • NiFe/SCFN delivers an ultra-low overpotential (19.2 mV @10 mA∙cm‐2) and shows excellent stability. [ABSTRACT FROM AUTHOR]