The energy industry is placing more and more emphasis on the need for effective and affordable electrocatalysts for hydrogen evolution reactions (HER). In this work, an iron-doped NiS/Ni(OH)2/CC composite material was synthesized by simple hydrothermal sulfurization processes of bimetallic Prussian blue analogue (PBAs) precursors grown in situ on three-dimensional (3D) Ni(OH)2 nanosheets. The overpotential can be 103 mV to attain current densities of 10 mA cm-2. The excellent catalytic activity of Fe-NiS/Ni(OH)2/CC is because of the unique 3D structure and the uniform doping of iron caused by the in situ growth of PBA, as well as the high conductivity of the self-supported electrode carbon cloth.