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Developing an environmentally friendly adsorbent with high adsorption capacity and economic advantages is crucial for the treatment of cadmium (Cd)-contaminated wastewater. In this study, Bentonite (Bt), which is widely distributed in nature, was used to prepare a new type of chitosan (CS)-grafted polymerized aluminum-pillared bentonite (i.e., Al@Bt): CS@Al@Bt. This new material effectively addresses the issues of chitosan's poor mechanical strength, limited load capacity, and the weak adsorption properties of raw bentonite for Cd. The effects of synthesis conditions on Cd adsorption by modified bentonite were investigated through batch experiments. The adsorption mechanism was revealed by characterization tests such as X-ray diffraction (XRD), N 2 adsorption-desorption experiments, Scanning and Transmission electron microscopy (SEM-TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The results showed that compared to raw Bt, when the ratio of Al in polymerized aluminum to the cation exchange capacity (CEC) of Bt was increased to 5 (i.e., Al/CEC=5), the specific surface area (SSA) of Bt increased from 78.46 m²/g to 195.99 m²/g. Additionally, the interlayer spacing and total pore volume increased by 1.22 and 1.13 times, respectively. After grafting chitosan onto Al@Bt, CS@Al@Bt reached adsorption equilibrium rapidly within 15 min, achieving a removal rate of up to 99.82% (initial concentration of Cd(II) was 20 mg/L, and the solid-liquid ratio was 1 g/L). Additionally, CS@Al@Bt showed good adsorption performance over a wide pH range. The rich pore structure of CS@Al@Bt and the complexation between amino (-NH 2) and hydroxyl (-OH) groups with Cd(II) were the main mechanisms for the removal of Cd(II) from the solution. The application showed that CS@Al@Bt effectively reduced Cd-containing mining wastewater from class V to class II quality, underscoring its significant potential for treating Cd(II)-contaminated wastewater. [Display omitted] • A modified bentonite (CS@Al@Bt) with efficient adsorption for Cd(II) was synthesized. • Higher polymerized aluminum content resulted in more micropores in CS@Al@Bt. • Chelation between -NH 2 , -OH, and Cd(II) played a dominant role in the adsorption. • CS@Al@Bt exhibited excellent adsorption properties for Cd(II) over a wide pH range. [ABSTRACT FROM AUTHOR]