a Well-aligned ZnO nanorods were uniformly coated with a layer of CuInS 2 nanoparticle photosensitizers using a tailored sequential pulsed electrodeposition. The formation of CuInS 2 -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.Owing to the distinct electron transport behaviour, one dimensional (1D) nanoarrays of photoactive oxide materials have attracted considerable attention in the design of photovoltaics, liquid state photoelectrochemical cells, and photocatalysis. which could be either highly ordered or randomly packed.3 To extend the light-response of these wide band gap 1D-nanostructured oxides, decoration with narrow bandgap materials as photosensitizers is a popular and effective strategy. 4 Although powders of these oxides can be conveniently coated with binary and ternary photosensitizers (e.g. CdS and CuInS 2 ) using hydro (solvo-)thermal method, 5 it remains a great challenge to directly cover the surface of the 1D-nanostructures in the thin film configuration. For thin films, electrodeposition is a simple and effective technique to decorate compact films with a wide range of metallic components, but due to the differences in the deposition kinetics and mechanisms, coating the arrays of wellaligned nanorod and nanotube thin films with secondary components always results in an inadequate coverage of the 1D-nanostructures, and it is mostly limited to the top layer (or entrance)of the 1D-nanostructures. A generally accepted reason is that a gradient of precursor concentration exists throughout the length of the 1D-nanostructures. Higher concentration of the precursor at the top region of the 1D-nanostructures induces rapid nucleation or deposition when cathodic bias is applied. This leads to the immediate formation of the secondary component at the top region (entrance), and subsequently blocks/slows the diffusion of fresh precursor into the deeper region for successive deposition. CuInS 2 is a visible-light-active semiconductor with a chalcogenide-type crystal structure. It demonstrates great potential applications in photovoltaic cells and solar hydrogen cells. 6 Unlike depositing binary sulphides, electrodeposition of the ternary sulphide CuInS 2 is more challenging because it involves multi elemental deposition. Therefore, the objective of this study is to uniformly deposit CuInS 2 nanoparticles on vertically aligned ZnO nanorod arrays grown on a transparent charge collecting electrode, i.e. fluorine-doped tin oxide (FTO) glass substrate. The formation of effective junctions between ZnO and CuInS 2 will allow superior charge transfer from the photoexcited CuInS 2 to ZnO upon illumination. The charges can be efficiently collected at the charge collecting electrode to improve the charge utilisation. Together with greater light penetration into deeper regions of the 1-D nanostructured film, the pulsed-electrodepos...