In this research, the zeolitic imidazolate framework 67 (ZIF-67) and carboxymethyl cellulose (CMC)/ZIF-67 biocomposite (CMC/ZIF-67) were synthesized. Different analyses were used to characterize the synthesized materials. Then, carboxymethyl cellulose and CMC/ZIF-67 biocomposite were used to remove the dye (Malachite Green: MG). The results showed that the dye removal capability of biocomposite (92.35%) is higher than that of carboxymethyl cellulose polymer (9.41%). As the adsorbent dose increases, the removal percentage of MG also increases. As the adsorbent dose increases, the active sites of the adsorbent surface are more accessible, and the dye removal percentage is higher. The dye removal percentage in 1, 2, 3, and 4 mg of composite adsorbent was 25, 54, 79, and 92.35%, respectively. With the increase in dye concentration, the amount of dye removal decreased. The dye removal in 20, 30, 40, and 50 mg/L concentrations with composite was 92.35, 85, 79 and 71%, respectively. The presence of imidazole rings in the structure of ZIF-67 as a ligand can be one of the main reasons for the high adsorption capacity of the biocomposite. Due to the double bonds in the imidazole rings, Π-Π stacking interactions occur with the aromatic rings of MG. This special interaction enables the biocomposite to adsorb the high capacity of MG. The isotherm and kinetics of dye adsorption by CMC/ZIF-67 biocomposite followed the Langmuir isotherm and pseudo-second-order kinetics.