In this study, CeO2 nanoparticles were synthesized by the sol–gel method using gelatine templates. The prepared CeO2 analyzed by analytical techniques displayed the fluorite structure with uniform sizes of 10–25 nm, a BET‐specific surface area of 65.8 m2/g, a pore volume of 0.144 cm3/g, and the existence of oxygen vacancies, suggesting their compatibility for adsorption removal of pollutants. The adsorption of arsenate and fluoride on CeO2 exhibited the maximal adsorption capacity of 224 and 64 mg/g, respectively. The kinetics of the adsorption fitted the pseudo‐second‐order model perfectly. Compared to fluoride, the adsorption of arsenate was found kinetically more but thermodynamically less favored. It can lie on the more stable complexes formed between arsenate and the prepared CeO2, the larger size of arsenate ions, and the mesoporosity of the prepared CeO2. As a result, the pore of the prepared CeO2 is filled quickly with arsenate ions, becoming full after a specific time that prevents the filling of further arsenate ions. Moreover, the CeO2 adsorbent demonstrated its high reusability up to 9 times without losing remarkable adsorption capacity (≤10%). Overall, the prepared CeO2 can be applied for the treatment of drinking water and wastewater in several regions of Vietnam.