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Constructing lightweight and porous adsorbents which can effectively remove dye contaminants is of great significance in the field of the sewage treatment. In this work, anisotropic cellulose nanofibril (CNF) composite sponges assisted by rectorites are fabricated through directional freeze-drying. The resulted composite sponge exhibits the superior saturated adsorption capacity and removal efficiency of 120.0 mg/g and 96.1% for methylene blue (MB), respectively, which is better than the pure CNF sponge and rectorite powders. This is attributed to the strong electrostatic interaction between CNFs and MB, and good cation exchange property of rectorites inside the three-dimensional (3D) highly porous composite sponge. The MB adsorption process of the composite sponge fits to the pseudo-second-order kinetic model and the Langmuir isotherm model well, which is affected by both boundary layer and intraparticle diffusion, resulting in a theoretical maximum adsorption capacity of 214.6 mg/g. Moreover, it also possesses a selective adsorption capacity for anionic and cationic dyes, which is expected to realize the separation treatment of different dyes according to actual application requirements. [Display omitted] • Anisotropic CNF/rectorite composite sponge by directional freeze-drying. • Superior MB adsorption capacity and removal rate of 120.0 mg/g and 96.1%. • Selective adsorption and separation capacity for anionic and cationic dyes. • Detailed evaluation of the adsorption behavior and mechanism. [ABSTRACT FROM AUTHOR]