Currently, there is a growing interest in the use of natural materials in various fields of science, technology and environmental protection due to their availability, low-cost, non-toxicity and biodegradability. Chitosan, natural clay of local origin, montmorillonite, zeolite, cross-linking agents (epichlorohydrin, sodium tripolyphosphate, glutaraldehyde) and plasticisers (glycerol) were used to synthesise composites. The composites were characterised by attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), X-ray diffraction analysis (XRD) and scanning electron microscope (SEM), tested for their antibacterial activity and used in batch experiments to study the adsorption of caesium, cobalt and europium ions. The maximum capacities for adsorption of caesium, cobalt and europium on the composites were 1400 mg/g, 900 mg/g and 18 mg/g, respectively. The experimental data fit better the Langmuir isotherm model and indicate favourable monolayer adsorption of Cs+, Co2+ and Eu3+ at homogeneous sites of the composites. The experimental data were in better agreement with the pseudo-second-order non-linear kinetic model for most elements and adsorbents. Adaptive neuro-fuzzy inference system proved to be a practical tool with good performance and generalisation capability for predicting the adsorption capacity of composites for caesium, cobalt, and europium ions. It was found that the predicted data were very close to the experimental data.