The growing concern regarding the environmental protection has encouraged researchers to focus their efforts on developing better and more effective possibilities of removing pollutants. In this research, a biocomposite adsorbent of covalently crosslinked chitosan-epichlorohydrin/coal fly ash (CHT-ECH/CFA) was synthesized and applied for reactive red 120 dye (RR120) removal. The CHT-ECH/CFA was characterized by BET, pH potentiometric, pHpzc, XRD, FTIR and SEM-EDX. Box–Behnken Design (BBD) was employed to assess the effects of the adsorption key parameters such as CFA loading into CTH-ECH matrix, adsorbent dose, solution pH, working temperature and contact time. The optimized CFA loading, adsorbent dose, temperature, time, and pH were observed to be 50 %, 0.07 g, 45 °C, 60 min, and pH 4 respectively. From BBD, the highest removal of RR120 removal at optimum conditions was found to be 90.2%. The results showed that adsorption performance can be modelled perfectly by both Langmuir and Freundlich isotherm models with maximum adsorption capacity of 237.7 mg/g at 45 °C. Moreover, the adsorption kinetics were well fitted to the pseudo-second order model. Based on the findings from the experiments conducted, the hybrid biocomposite adsorbent offers adequate potential for the treatment of anionic dye-polluted water.