The development of composite adsorbent coating based acrylic polymer solution (APS) mixed with bentonite (ben) was investigated. The composite adsorbent coating was prepared and coated to a high surface area substrate, cotton cellulosic fiber (CCF). The APS/ben-CCF was used for a single cationic methylene blue (MB) dye adsorption system. Characterization of composition and structure of materials and coating was carried out by X-ray fluorescence (XRF), scanning electron microscopy (SEM), and UV-spectroscopy (UV-VIS). The adsorption properties of the APS/ben-CCF were investigated as a function of solution pH, initial dye concentration and contact time as well as solution temperature of MB dye. The result revealed that the APS/ben-CCF functioned well in solutions of various pH (acidic to alkaline), achieving 100% removal of MB within 2 hours of adsorption for 50 ppm. Kinetic studies showed that APS/ben-CCF is endothermic in nature since the adsorption capacity increased with increasing solution temperature. These results demonstrate that APS/ben-CCF composite adsorbent coating is an advanced adsorbent with advantages such as easy phase separation and capability to remove cationic dyes in a short time period