ZnO, In2Cu2O5, and ZnO/In2Cu2O5 have been synthesized using Gardenia jasminoides Ellis leaf extract, which contains essential secondary metabolites. Modification of ZnO with In2Cu2O5 and their photocatalytic activity was explored for the first time under visible light irradiation ZnO/In2Cu2O5 nanocomposite possessed the decrement of band gap energy of ZnO to 2.84 eV, which was more susceptible to visible light. TEM analysis validated that the average size of ZnO/In2Cu2O5 particles was approximately 50.45 nm, suggesting the formation of a composite material in a nanoscale. For the photocatalytic evaluation, 5 mg of ZnO/In2Cu2O5 nanocomposite degraded malachite green dye for 120 min with an efficiency of 93.91%. The photocatalytic properties of ZnO/In2Cu2O5 were superior to those of ZnO and In2Cu2O5. The notable increase in photocatalytic activity was due to the faster reaction rate. The present study demonstrates that visible-light ZnO-based materials with a small amount are efficient environmental photocatalysts, such as dye degradation.