Wastewater from industries contributes significantly to pollution. Adsorption of acidic dye using by nanohybrid biopolymeric hydrogels has evolved as one of the viable techniques. Graphene oxide (GO)/chitosan (CS)–polyvinyl alcohol (PVA), GO/starch–PVA, and GO/agar–PVA hydrogels were synthesized. The results revealed that the following results are the ideal values: GO/CS–PVA: 3 pH (8.251 mg g−1), 0.05 g/50mL dosage (8.251 mg g−1), 90 min (8.251 mg g−1), 12 ppm dye concentration (8.251 mg g−1), and 30 °C (8.251 mg g−1); for GO/starch–PVA: 2 pH (7.437 mg g−1), 0.05 g/50 mL dosage (7.437 mg g−1), 90 min (7.437 mg g−1), 12 ppm dye concentration (7.437 mg g−1), and 30 °C (7.437 mg g−1); and for GO/agar–PVA; 3 pH (6.142 mg g−1), 0.05 g/50 mL dosage (6.142 mg g−1), 90 min (6.142 mg g−1), 12 ppm dye concentration (6.142 mg g−1), 30 °C (6.142 mg g−1). GO/CS–PVA outperformed the other hydrogels. The Langmuir model suited GO/CS–PVA data, while GO/starch–PVA and GO/agar–PVA hydrogels followed Freundlich isotherm models. The adsorption capacity data followed a pseudo-second-order model. Negative value of Gibbs free energy and enthalpy showed that the reactions were spontaneous and exothermic in nature. The presence of heavy metals, electrolytes, and detergents/surfactants affected the dye adsorption. Entropy changes positive values implied that randomness raised at the solid/solution contact. The desorption (60, 55, and 58%) of GO/CS–PVA, GO/starch–PVA, and GO/agar–PVA hydrogels was obtained using 0.5 N NaOH. Scanning electron microscope, X-ray diffraction, and Fourier transform infrared (FT-IR) were used for characterization.