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Indigo carmine in aqueous solution was effectively degraded using ZnO-Bi2O3/Graphitic Carbon Nitride heterojunction structure by visible light/H2O2 system. The mechanism of photocatalytic degradation of Indigo carmine shows the responsible species for the degradation of Indigo carmine in the ZnO-Bi2O3-xC3N4/H2O2/visible light system (x = 0, 1, 2, and 3) is the hydroxyl radicals which were generated from the reaction of e− and h+ with H2O2. Under optimal conditions, ZnO-Bi2O3-2C3N4/H2O2/Vis system degraded more than 93% of Indigo carmine in 180 min. Besides, the kinetic of the photocatalytic process was detailed. These results demonstrate that the ZnO-Bi2O3-2C3N4/H2O2/visible light system may become a promising approach to achieve efficient environmental remediation as an environmentally friendly oxidant. Keywords: Indigo carmine, Hydroxyl radicals, Photocatalyst, Degradation, Mineralization