It is still strongly required to explore non-noble catalysts with excellent performances for hydrogen generation. MoP-based catalysts are demonstrated as good candidates and further improvements are highly encouraged. Herein, a novel strategy of N-doping has been proposed to increase the HER performance over the MoP-based catalysts, in which nitrilotriacetic acid (N(CH2COOH)(3), NTA) is selected to provide the doping element of N. With the addition of NTA, the N-doped MoP catalysts with good distribution have been successfully prepared, showing smaller particle size, reduced electrical resistance, increased amount and better quality of active sites, resulting in much better performances compared to pure MoP. This strategy can also be extended to other counterparts for the further improvement of HER activity by N-doping. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.