The novel graphene oxide-ionic liquid grafted chitosan composites (denoted as GO-ILCS) are firstly prepared via a self-assembly process. Then, they are used to anchor ultrafine palladium nanoparticles by the in-situ reduction of palladium chloride with sodium borohydride. The resultant Pd(0)/GO-ILCS organic-inorganic hybrid catalysts are characterized by various techniques and used to catalyze the hydrolytic dehydrogenation of ammonia borane (NH3BH3, AB) under ambient conditions. The results reveal that the palladium nanoparticles are highly dispersed on GO-ILCS and the Pd(0)/GO-ILCS catalysts exhibit high catalytic activity and excellent reusability in the reaction. The turnover frequency (TOF) is as high as 25.6 mol(H2), center dot mol(Pd)(-1)center dot min(-1) and the catalytic activity does not decrease obviously after six runs. The orders of palladium and AB concentrations are 1.00 and 0.33 in the catalytic reaction, respectively. Notably, the activation energy of the reaction (Ea = 38 kJ mol(-1)) over the resultant catalysts is obviously lower than most of the palladium-based catalysts reported previously. It is expected the Pd(0)/GO-ILCS catalysts are of exciting potential in the field of hydrogen energy. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.