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In this paper, we report the fabrication of ionic liquid (IL)-modified molybdenum disulfide (MoS2) composites via a simple but effective method, that relied on Gamma-ray-initiated polymerization of polydopamine (PDA) modified MoS2 nanosheets using IL as a monomer. The adsorptive removal of Congo red (CR) from aqueous medium by MoS2@PDA@IL composites was investigated. Batch experiments were carried out thoroughly to explore the effects of various experimental factors, such as contact time, containment initial concentration, and the function of pH and system temperature on the adsorption of MoS2@PDA@IL composites towards CR. Based on the experimental data, the adsorption kinetics, isotherms (Langmuir and Freundlich) and thermodynamics were also studied. We demonstrated that the adsorption of CR on MoS2@PDA@IL is a spontaneous and endothermic process. The amount of adsorbed CR of the MoS2@PDA@IL composites (Qe, max = 112.16 mg/g) is 2.77 times that of pristine MoS2 (Qe, max = 40.54 mg/g). The above results demonstrated that PIL functionalized MoS2 nanosheets are promising for adsorptive removal of environmental pollutants. More importantly, owing to the universal adhesion capability of polydopamine, the method might also be extended for the fabrication of other polymeric composites with different functions for various applications. Therefore, this work will attract interest from scientists in the materials, chemistry and environmental fields.