This study focusses on the synthesis of chitosan-cellulose composite membrane derived from Labeo rohita fish scales (FS) for the removal of Cr(III) from aqueous solution, while chromium is a serious threat to groundwater. Waste FS are valorized to chitosan by demineralization, deproteination, and deacetylation successively. Cellulose was extracted from sugarcane bagasse using acidic hydrolysis. Chitosan-based cellulose composite porous membrane was fabricated by evaporating solvent from polymer solution in petri dish. The impact of pH, contact time, and absorbent dosage on the removal of Cr(III) from an aqueous solution was investigated. Atomic absorption spectrophotometer was used to check the Cr(III). Results showed that chitosan comprising 85% degree of deacetylation was achieved by alkali treatment, while yield was 22%. FTIR analysis confirmed the chitosan and chitosan-cellulose-based composite membrane. Morphology studies showed that the cellulose was strongly staggered and due to the chitosan, the surface of cellulose became rougher, which is good to enhance the adsorption capacity. The maximum removal 57% of Cr(III) from aqueous solution was observed at pH 6 at 60 min and 50 mg dosage of adsorbent. The minimum removal (47%) of Cr (III) was found at pH 2. These results confer that Labeo rohita-based chitosan-cellulose composite membrane has great potential for the removal of metals from industrial effluents.