Carbon quantum dots/bimetal phosphide (CQDs@NiCoP) catalysts for electrocatalytic hydrogen evolution reaction were synthesized via a facile annealing method. In a 0.5 M H2SO4 system, the 30 mg/L CQDs@NiCoP catalyst performed well with high electrocatalytic activity, lower initial overpotential than pure NiCoP (108 vs. 182 mV) and lower Tafel slope of 80 mV/decade. The enhancement of hydrogen evolution reaction activity was probably because the addition of CQDs enhanced the catalyst conductivity and significantly accelerated charge transfer.