Well-aligned ZnO nanorods were uniformly coated with a layer of CuInS2 nanoparticle photosensitizers using a tailored sequential pulsed electrodeposition. The formation of CuInS2-ZnO heterojunction with well-matched band energy alignment and the superior electron mobility in ZnO nanorods led to a remarkable 3.75 times improved photoelectrochemical performance of the electrode under visible light irradiation.