Due to their toxicity, the removal of heavy metal contaminants, particularly from aqueous solutions, is an important issue for the remediation field. This paper describes the performance of photocatalytic reduction of hexavalent chromium (Cr [VI]) using clinoptilolite as a natural zeolite (Ze) modified by titanium dioxide (TiO2 or Ti) and polyoxypropylene (POP) surfactant. The removal efficiency of the modified Ze was evaluated in the presence of Ze–Ti–POP and Ze–Ti nanocomposites under UV‐A irradiation and visible light. The effects of different factors including contact time (0–330 min), adsorbent dose (2, 4, 6, 8, and 10 g/L), initial pH (1, 2, 3, 4, and 5), and initial Cr (VI) concentration (5, 10, 15, 20, and 25 mg/L) were studied. The results showed that maximum removal efficiencies of Cr (VI) by Ze–Ti and Ze–Ti–POP nanocomposites in the optimum experimental conditions (i.e., contact time: 30 min, dose: 10 g/L, pH: 2, initial concentration: 10 mg/L) under UV‐A irradiation were 88% and 97%, while the corresponding reductions for visible light were 80% and 91%, respectively. Adsorption kinetics data fit well with the pseudo‐second‐order model. Furthermore, reusing nanocomposites after three regeneration cycles revealed that the application of Ze–Ti and Ze–Ti–POP nanocomposites could be a promising approach for removing Cr (VI) from aqueous solutions.