This research article presents the fabrication of NH₂-terephthalic acid crosslinked chitosan-bentonite composite, which adopted a facile synthesis approach and offered efficient adsorption capacity for organic dyes. A novel hydrogel material named CB 5:1 demonstrated remarkable adsorption for anionic dyes (Congo red (CR) and brilliant blue (BB)) while showing a negligible affinity for cationic dyes. Adsorption isotherm studies revealed the adsorption capacity of 4950 mg/g and 2053 mg/g (per g of composite's dry weight) for CR and BB following the Langmuir adsorption model. Kinetics and thermodynamic studies were also conducted while the adsorption of anionic dyes in the presence of metal ions, cationic dyes, anionic dyes, and in simulated water remained unaffected. Laccase, an industrially important enzyme, was also immobilized on CB 5:1 to achieve enzyme stability and reusability, resulting in a staggering immobilization capacity (4782 mg/g) at pH 6.0. Laccase immobilized product was employed to perform dye degradation (> 90 % for CR and > 75 % for BB), and the reusability was tested. Overall, our crosslinked product proved appealing for removing high concentrations of anionic organic dyes from polluted water and could be envisaged for practical use.