The cost-effective removal of heavy metal ions represents a significant challenge in environmental science. In this study, we developed a straightforward and efficient reusable adsorbent by amalgamating chitosan and vermiculite (forming the CSVT composite), and comprehensively investigated its selective adsorption mechanism. Different techniques, such as Fourier-transform infrared spectroscopy (FTIR), zeta potential analysis, scanning electron microscopy (SEM), X-ray diffraction (XRD), and Brunauer, Emmett, Teller (BET) analysis were employed for this purpose. The prepared CSVT composite exhibited a larger surface area and higher mesoporosity increasing from 1.9 to 17.24 m2/g compared to pristine chitosan. The adsorption capabilities of the CSVT composite and pristine chitosan for Cu(II) and Cd(II) species were systematically examined. Due to its porous structure and increased surface area, the CSVT composite demonstrated superior adsorption ability when compared to pristine chitosan. The maximum adsorption capacities of Cu(II) and Cd(II), determined by Langmuir adsorption isotherms in batch experiments, were found to be 116.22 and 147.64 mg/g, respectively, under initial pH conditions of 8 and an initial concentration of 250 mg/L. The thermodynamic analysis revealed that the adsorption process for both metal ions is spontaneous, endothermic physisorption, and thermodynamically favorable. These findings collectively affirm the CSVT composite as a highly promising adsorbent for the efficient and selective removal of Cu(II) and Cd(II) from aqueous solutions