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The development of high activity, low-cost and stability hydrogen evolution reaction (HER) catalysts is a core issue in the field of water splitting. Herein, the bimetallic CoMo MOFs-derived N-doped carbon nanospheres with Co/Mo–N bonds is proposed to effectively improve the electrocatalytic HER performance. Meanwhile, the combination of the porous and spherical structure further promotes the effective contact on the electrode/electrolyte interface while enhancing the electrolyte into the inner structure of the material for a fast HER process. In addition, the N-doped and bimetallic Co/Mo oxides on the rough surface of nanospheres have the capability to furnish more electrocatalytic active sites. The obtained electrocatalyst owns the small overpotential of 112 mV at 10 mA cm−2 and Tafel slope of 106.8 mV dec−1 in 1.0 M KOH solution. This work provides a new prospect for the rational design and fabrication of bimetallic active sites in carbon nanomaterials electrocatalysts in the relevant energy applications. [Display omitted] • Bimetallic CoMo MOFs-derived N-doped carbon nanospheres is proposed to effectively improve the electrocatalytic HER performance. • The formation of Co–N and Mo–N, which would provide a fast electron transfer path in electrocatalytic process. • The formation of CoO and CoMoO 3 species could synergistic promote the adsorption and reaction of the H ads intermediates. [ABSTRACT FROM AUTHOR]