This study was directed to use the sugarcane bagasse wastes as bio-sorbent materials to remove cationic dyes; Methylene Blue (MB) and Crystal Violet (CV), from synthetic industrial wastewater. The collected and dried sugarcane bagasse wastes were treated with different concentration of H2SO4 as a pre-treatment step in the production of bioethanol after hydrolyzing the lignin content. Afterwards, the unhydrolyzed wastes were dried and ground with a ball mill then mixed with cellulose acetate to form composite sheets that directed to biosorption process. The composite sheets were functionally and structurally explored using FT-IR, XRD, SEM, swelling and the porosity. Optimization of the biosorption processes were performed using “One Factor at A Time (OFAT)" and subsequently “a full factorial design". Results displayed that, the MB removal efficiency of 90.36% was accomplished using a composite sheet dose of 5 g/l treated with 4% H2SO4 for 100 ppm MB after 240 min. In addition, the CV removal efficiency of 89.29 % was obtained by using the same composite sheet with dose of 7g/l for removing of 500 ppm CV after 240 min. Isotherms and Kinetics models were also examined. Moreover, the reusability experiment was demonstrated for 5-times use. In conclusion, the unhydrolyzed sugarcane bagasse wastes, that remained after treated with different sulfuric acid concentrations, combined with cellulose acetate were successfully provide different composite sheets that applied in the 3Rs processes, Removal, Recover and Reuse of the MB and CV dyes.