In this study, tunable Schiff's base-cross-linked chitosan-glutaraldehyde (CS-GLA) was modified and applied to remove reactive red 120 (RR120) dye from an aqueous solution. Different ratios of TiO2 nanoparticles, such as 25% TiO2 nanoparticles (CS-GLA/TNC-25) and 50% TiO2 nanoparticles (CS-GLA/TNC-50), were loaded into the CS-GLA's molecular structure. The adsorptive properties of CS-GLA, CS-GLA/TNC-25, and CS-GLA/TNC-50 for the RR120 dye in the aqueous solution were evaluated. CS-GLA/TNC-25 exhibited the best adsorptive property possibly because of the perfect balancing between the surface area and available amine (NH2) groups in the composite formulation. The impact of adsorption key parameters, such as adsorbent dosage (0.01-1.2 g), RR120 dye concentration (30-400 mg/L), solution pH (3-12), and contact time (0-400 min) were explored by batch adsorption mode. The adsorption was well described by the Freundlich model and pseudo-second order kinetic model. The adsorption capacity of CS-GLA/TNC-25 for RR120 dye was 103.1 mg/g at 303K. The adsorption mechanism of RR120 on the CS-GLA/TNC-25 surface can be assigned to various interactions, such as electrostatic attraction, n-π stacking, and H-bonding. Results indicate the potential application of CS-GLA/TNC-25 as environment-friendly biosorbent for removing acid and/or textile dyes, such as RR120, from aqueous environments.