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Graphene oxide has been widely used in the oxidative degradation of environmental pollutants. However, its catalytic role can be questioned as graphene oxide with oxygen-containing functional groups may also act as reactant in oxidative reactions. Herein, hydrogel composites loaded with multilayered graphene platelets showed excellent catalytic performance for the reduction of a wastewater organic pollutant (methylene blue) under NaBH₄, which proved the catalytic role of multilayered graphene platelets. The liquid-based direct exfoliation method was used to prepare two-dimensional materials, which is compatible with other liquid phase methods to prepare nanomaterials. Hydrogel composites composed of multilayered graphene platelets, silver nanoparticles, and polyacrylic acid hydrogels were synthesized in water solution under irradiation with ultraviolet light, demonstrating the advantages of synthesizing nanocomposites using the liquid-based direct exfoliation method.