Graphite carbon nitride (g-C 3 N 4 ) supported PtNi alloy nanoparticles (NPs) were fabricated via a facile and simple impregnation and chemical reduction method and explored their catalytic performance towards hydrogen evolution from ammonia borane (AB) hydrolysis dehydrogenation. Interestingly, the resultant Pt 0.5 Ni 0.5 /g-C 3 N 4 catalyst affords superior performance, including 100% conversion, 100% H 2 selectivity, yielding the extraordinary initial total turnover frequency (TOF) of 250.8 mol H2 min −1 (mol Pt ) −1 for hydrogen evolution from AB at 10 • C, a relatively low activation energy of 38.09 kJ mol −1 , and a remarkable reusability (at least 10 times), which surpass most of the noble metal heterogeneous catalysts. This notably improved activity is attributed to the charge interaction between PtNi NPs and g-C 3 N 4 support. Especially, the nitrogen-containing functional groups on g-C 3 N 4 , serving as the anchoring sites for PtNi NPs, may be beneficial for becoming a uniform distribution and decreasing the particle size for the NPs. Our work not only provides a cost-effective route for constructing high-performance catalysts towards the hydrogen evolution of AB but also prompts the utilization of g-C 3 N 4 in energy fields.