A novel dual-templating method was developed to prepare N-doped carbon nanosheets with a similar microstructure but a broad N-doping level (from 0 to 21.6 at%) as support for Ni nanoparticles for the hydrogen oxidation reaction (HOR). It is found that the HOR activity on the catalysts exhibits a volcano dependence on the N content of carbon nanosheets, probably due to the change in the hydrogen binding energy on the surface Ni nanoparticles induced through N doping. The catalyst with an N content of 8.7 at% exhibits an optimal HOR activity, which is even comparable to some Pt-group catalysts.