A novel Chitosan/Indium sulfide (CS/In2S3) nanocomposite was created by co-precipitating Chitosan and InCl3 in solution, resulting in In2S3 agglomeration on the Chitosan matrix with a remarkable pore diameter of 170.384 Å, and characterized it for the physical and chemical properties. Under optimal conditions (pH = 7, time = 60 min, catalyst dosage = 0.24 g L−1, and dye concentration = 100 mg L-1), the synthesized nanocomposite demonstrated remarkable adsorption capabilities for Victoria Blue (VB), attaining a removal efficiency of 90.81%. The Sips adsorption isotherm best matched the adsorption process, which followed pseudo-second-order kinetics. With a rate constant of 6.357 × 10–3 g mg−1 min−1, the highest adsorption capacity (qm) was found to be 683.34 mg g−1. Statistical physics modeling (SPM) of the adsorption process revealed multi-interaction and multi-molecular adsorption of VB on the CS/In2S3 surface. The nanocomposite demonstrated improved stability and recyclability, indicating the possibility for low-cost, reusable wastewater dye removal adsorbents. These results have the potential to have practical applications in environmental remediation.