The electrocatalytic activity for hydrogen evolution reaction (HER) is strongly correlated with active edge sites and resulting efficient charge transport capability. Here, we presented a facile two-step method to synthesize 3D hierarchical NiS2/MoS2 composite nanostructures on a carbon fiber paper (CFP) skeleton. The nanostructures distributed on CFP uniformly and composed of 2D nanosheets, which would provide plenty of active edge sites and increase the HER activity. Electrochemical measurement suggests that the prepared NiS2/MoS2 exhibit great HER activity including a low overpotential of 102 mV, a small Tafel slope of 67 mV/dec, and a high double-layer capacity of 53.7 mF/cm2 in 1 M KOH aqueous solution. In addition,the HER activity is almost unchanged after galvanostatic technique with applied current densities of 10 mA/cm2 for 20 h.