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The tunable photo-induced electronic property of the Cs2[{Mo6Bri8}Bra6] and Br2[{Ta6Bri12}(H2O)a6] octahedral metal cluster-based compounds was characterized by the zeta potential measurement upon irradiation by ultraviolet–visible (UV–Vis) light. The enhancement of the electronic charge on the surface of the [{Mo6Bri8}Bra6]2- cluster-based anion caused by the irradiation increased the negative zeta potential. Both compounds showed the dependence of the zeta potential as a function of the light excitation. This will be a promising property for sensor applications based on the reversibility of the photo-electrochemical properties of the functional cluster.