The novel composites consisting of graphitic carbon nitride and chitosan (denoted as g-C3N4-CS) is synthesized for anchoring palladium nanoparticles. The results reveal that the resultant catalysts possess superior catalytic activity for ammonia borane (AB) hydrolysis. The corresponding turnover frequency reaches up to 27.7 molH2 center dot molPd-1 center dot min-1at 30.0 degrees C, and the activation energy is as low as 35.3 kJ mol(-1). Kinetics study reveals that the hydrolysis reaction is 0.50 and 0.68 orders with AB concentration and palladium concentration, respectively. In addition, the catalytic activity of the resultant Pd(0)/g-C3N4-CS catalysts is stable even after 10 runs. The result will be helpful for the development of hydrogen generation and functional materials.