Abstract: To address the heavy metal pollution in mine wastewater and overcome the drawbacks of conventional powdered adsorbents such as easy loss and difficult separation, recyclable spherical Na-P molecular sieves were prepared using kaolin as raw material via alkali modification, hydrothermal crystallization combined with cross-linking forming process. The adsorption behavior and mechanism of the as-prepared adsorbent toward Cd²⁺ and Fe³⁺ in mine wastewater were systematically investigated. The structural properties of the material were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy dispersive spectroscopy (EDS), Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS).The results show that the spherical kaolin-based molecular sieves exhibit a stable three-dimensional porous structure and retain the complete crystal framework of Na-P molecular sieves after cross-linking forming. The optimal adsorption pH for both Cd²⁺ and Fe³⁺ is 6. The maximum adsorption capacities were 19.29 and 19.89 mg·g^-1 .The adsorption process complies with the pseudo-second-order kinetic model and Langmuir isotherm model, indicating that the adsorption is dominated by chemical adsorption and monolayer adsorption. In the binary competitive adsorption system, Fe³⁺ shows stronger competitive adsorption capacity, preferentially occupying active sites and inhibiting the removal of Cd²⁺. Mechanism analysis reveals that the removal of Cd²⁺ and Fe³⁺ is mainly attributed to ion exchange, electrostatic attraction, and surface complexation.Recycling experiments demonstrate that the removal efficiencies of Cd²⁺ and Fe³⁺ by spherical kaolin-based molecular sieves remain above 80% after 5 adsorption–desorption cycles, suggesting that the spherical three-dimensional framework significantly improves the structural stability and reusability of the material. Compared with traditional powdered molecular sieves, the spherical kaolin-based molecular sieves not only maintain adsorption activity but also enhance recyclability and engineering applicability, showing promising application prospects in the treatment of heavy metal-contaminated mine wastewater.