Kaolinite-rich soils were used to prepare zeolite-based composites via alkaline activation. The porous material was characterized by conducting XRD and microporosity measurements, as well as ESEM microscopy. The Weber and Morris (W-M) model was used for studying adsorption kinetics of radioactive cations on synthesized alkali-activated material. These investigations evidenced the effects of pore structure and the importance of the intrinsic characteristics of hydrated cations (ionic potential; hydrated radius; B-viscosity parameter; molar Gibbs energy of hydration of cation) on W-M kinetic rate constants. The application of diffusion-based models permitted us to assess the key diffusion parameters controlling successive diffusion regimes, and to reveal strong contributions of surface diffusion to adsorption kinetics during the course of the second and third kinetics stages of the W-M model. The magnitude of the surface diffusion coefficient was related to the capacity of hydrated cationic species to lose water molecules when penetrating brick pores. The HSDM model were tested for predicting radionuclide adsorption in a fixed-bed column. A breakthrough curve simulation indicated the predominance of the surface diffusion regime, which was in agreement with mathematical analysis of (batch) adsorption kinetics data. Ionic diffusion was linked to the characteristics of capillary porosity and connectivity of capillary pores in the composite, suggesting the generation of hydrated nuclides and their immobilization in the form of outer-sphere complexes.