A mesoporous crosslinked chitosan-activated clinoptilolite biocomposite (CS-GA/ACP) was prepared with chitosan (CS) as the substrate and glutaraldehyde (GA) as the crosslinking agent. Structural analysis of the CS-GA/ACP composite beads was performed using FTIR, SEM, and BET techniques. The adsorption properties of the CS-GA/ACP for Congo red (CR) and methylene blue (MB) removal were examined using a batch method. The effects of CS loading, CS-GA/ACP dosages (0.005-0.25 g), pH values (3-11), initial concentrations (30-300 mg/L), contact time (5-120 min), ionic strength, and temperatures (25-65 ℃) on the adsorption of CR and MB on the CS-GA/ACP composite beads were investigated. The pseudo-second-order kinetics could better describe the adsorption process than the pseudo-first-order kinetics, and the Langmuir isotherms model agreed well with the experimental data. The maximum adsorption capacities of the CS-GA/ACP for CR and MB were 180.59 mg/g and 143.67 mg/g at 25 ℃, respectively. The proposed mechanism studies showed that the possible interaction between the adsorbent and dye molecules were Yoshida H-bonding, dipole-dipole H-bonding, electrostatic interaction and n-π interaction. The CS-GA/ACP can be recycled to remove dyes without significant loss of efficacy, and the adsorption of dyes on the CS-GA/ACP is spontaneous endothermic adsorption. Overall, the CS-GA/ACP showed an excellent performance for dyes removal in aqueous solution and could be a practical candidate for industrial applications.