Here, reduced graphene oxide (RGO) supported surfactant free, RuNi alloy nanoparticles with particle size < 5 nm were synthesized by chemical coreduction route. The synthesized sample was well characterized by various techniques and showed complete solid solution without any extra phase, where Ru lattice is required for nucleation of metallic Ni. The Ru x Ni 100-x /RGO (x = 100, 75, 50 and 25) nanocomposites (NCs) exhibits remarkable activity in hydrolytic dehydrogenation of NH 3 BH 3 (ammonia borane, AB). Among various Ru x Ni 100-x compositions, Ru 50 Ni 50 NPs showed best performance with maximum H 2 evolution rate 9305.6 mL min À1 g À1 and TOF value 236 min À1 at 30 o C, which is one of the best value reported till date. In addition, present activity retained upto 7 th catalytic cycles, showing high durability which makes it a potential candidate for development of NH 3 BH 3 as a H 2 storage material. Moreover, alloy NCs further explored in tandem reduction of nitro and nitrile compounds in presence of AB as H 2 source which again showed best performance with excellent yield (> 99 %) of amine product with short time period of 4.5-10 min. Additionally, NCs exhibits high chemoselectivity and durability towards such organic transformation reactions. This high catalytic efficiency of RGO supported RuNi NPs could be ascribed to synergistic interaction between Ru/Ni metals, high surface area (small sized NPs and graphene sheets), RGO as a support material which prevent agglomeration of particle.