Our objective in this study is to fabricate a novel chitosan-based ternary nanocomposite hydrogel film by incorporating graphene oxide (GO) nanosheets into a chitosan/partially hydrolyzed polyacrylamide (PHPA) network to boost adsorption efficiency through one step self-assembly process in water. Basically, H-bonding interactions drive the formation of a crosslinking network structure. The Batch adsorption experiments evaluated the hydrogel nanocomposite's MB adsorption performance. By loading GO, surface roughness, swelling percentage (from 21,200 % to 35,800 %), elastic modulus of up to 73.7 Pa, and adsorption characteristics (from 282 mg/g to 468 mg/g) were enhanced. The nanocomposite displayed outstanding thermally/pH responsiveness properties. MB adsorption equilibrium was reached after 45 min and the adsorption capacity was 476.19 mg.g−1 when the initial concentration was 100 mg/L. The MB adsorption kinetics and isotherms by the nanocomposite were well correlated by the PSO and the Langmuir models (R2 > 0.99), respectively. The loaded nanocomposite was shown to be regenerative for five cycles through desorption studies. Thermodynamic analysis indicated that MB adsorption occurred spontaneously (ΔG°: −16.47 kJ/mol, 303 K) and exothermically (ΔH°: −79.49 kJ/mol). A plausible adsorption mechanism was proposed for the nanocomposite developed for MB removal. Our results can contribute to the design and fabrication of nanocomposite adsorbents to treat wastewater.