In order to develop a novel and cost-effective adsorbent with outstanding adsorption capacity and excellent recyclability for anionic pollutants, the chitosan-modified cetyltrimethylammonium bromide sorbent (CS@CTAB) was fabricated. Fourier-transform infrared spectroscopy, N2 adsorption–desorption isotherm, elemental analysis, Thermogravimetric analysis, X-ray diffraction, and Scanning electron microscopy have been applied to evaluate both raw and surfactant modified chitosan (CS@CTAB). Azorubine, Sunset Yellow, and hexavalent chromium were used to study the adsorption behavior of CS@CTAB under various parameters such as adsorbent dose, initial dye and metal ion concentration, contact time, and temperature. Adsorption equilibrium, kinetics models and thermodynamic parameters were investigated. The adsorption isotherm fitted well with the Langmuir isotherm model, with a maximum adsorption capacity of 492.6 mg/g, 492.6 mg/g, and 490.196 mg/g for Azorubine, Sunset Yellow, and Hexavalent Chromium, respectively. The kinetic studies showed that the pseudo-second-order model provided a better correlation between experimental data. Furthermore, the calculated thermodynamic parameters confirmed that the adsorption of Cr(VI), E110, and E122 by CS@CTAB material is a spontaneous and exothermic process. The fabricated CS@CTAB adsorbent was employed for the efficient elimination of Azorubine, Sunset Yellow, and hexavalent chromium from real water samples, synthetic mixtures, and colored soft drinks, with a percentage of recovery of ~ 96%. The plausible adsorption mechanisms of Azorubine, Sunset Yellow, and hexavalent chromium on the surface of CS@CTAB are elucidated. The adsorption anticipated to be due to electrostatic interaction and hydrogen bond formation for hexavalent chromium; while the adsorption of Azorubine and Sunset Yellow, was assumed to be due to electrostatic interaction, hydrogen bonding, and n-π interaction. Finally, the study demonstrates the efficiency of CS@CTAB for the removal of anionic species from several samples, including natural water and colored beverages.