Abstract: Cellulose nanofiber(CNF) was used as raw material, and then was blended with the modified montmorillonite(MMT) by cetyltrimethylammonium bromide(CTAB) to prepare CTAB@MMT-CNF. The effect of CTAB dosage on the properties of CTAB@MMT-CNF was explored, and CTAB@MMT-CNF was characterized by FT-IR, morphology analysis and thermal gravimetric analysis. Subsequently, the effects of composite and their dosage, and the concentration of methylene blue on the removal performance of methylene blue were investigated. The results showed that the dosage of CTAB would affect the compounding of CNF and CTAB@MMT, and more CNF would insert into the interlayer structure of MMT with 20% CTAB. It was also found that CTAB@MMT-CNF showed the best removal performance and the highest removal efficiency of methylene blue of 99.94% when 10 mL methylene blue solution(600 mg/L) was treated with 25 mg CTAB@MMT-CNF, in which the dosage of CTAB was 15%. Otherwise, this process was accorded with pseudo first order rate equation, its apparent constant was 0.025 7 s^-1 and the correlation coefficient was 0.965 3.