Carbon and nitrogen nanosheets (CN) were synthesized by the molten salt method using melamine as the precursor and lithium chloride as the templating agent, and the cyclic phosphonitrile-containing polymer carrier (POM) was synthesized by the solvothermal method using hexachlorotrisphosphononitrile and 2,6-diaminopyridine as the reactant, tetrahydrofuran as the solvent, and a certain amount of triethylamine was added to it, and the two were mixed to obtain the composite carrier with a two-dimensional laminar structure using the molten salt method and solvothermal method (POM-CN), and a series of NiCu/POM-CN catalysts were prepared by impregnation reduction method using POM-CN as the carrier. Based on TEM, SEM, XPS, XRD, FT-IR and UV-vis DRS characterization, the microstructures of the catalysts were analyzed, and the effects of the catalyst morphology and structure as well as photocatalysis on the hydrolysis performance of ammonia-borane (AB) for hydrogen production were investigated. The experimental results showed that under the irradiation of visible light, the TOF value of Ni0.4Cu0.6/POM-CN catalyst was as high as 1774.6 h-1, which was 2.8 times higher than that of the TOF value under the condition of no visible light (618.1 h-1), indicating that the catalyst had a good photocatalytic performance. Meanwhile, the catalyst still maintained a high catalytic activity after five cycle tests. In addition, the activation energy of the Ni0.4Cu0.6/POM-CN catalyst for the reaction in the presence of light was 52.75 kJ?mol-1. The characterization results indicated that the catalysts possessed excellent catalytic activity thanks to the POM-CN composite carrier, the alloying effect of the NiCu bimetal, and the strong interactions between the metal and the carrier.