The urgent need for clean and storable energy drives many currently topical areas of materials research. Among the many materials under investigation zinc oxide is one of the most studied in relation to its use in photo-(electro)chemical applications. This study aims to give an overview of some of the main challenges associated with the use of zinc oxide for these applications: the high density of intrinsic defects which can lead to fast recombination, low visible light absorption and the occurrence of photo-corrosion. Employing simple low-temperature solution based methods; it is shown how defect-engineering can be used to increase the photoelectrochemical performance and how doping can strongly increase the visible light absorption of zinc oxide nanorod-arrays. Furthermore the deposition of ultra-thin titanium dioxide layers using atomic layer deposition is investigated as possible route for the protection of zinc oxide against photo-corrosion. As one of the most studied metal-oxides Zinc Oxide (ZnO) has already found its way into many industrial applications. Nevertheless enormous research interest is still focused on this earth-abundant, environmentally-friendly material as it offers interesting material properties such as a high exciton binding energy, a direct bandgap and comparably high charge carrier mobility.1 Furthermore the ability to grow ZnO nanostructures using a wide range of deposition techniques offers new perspectives for the material to be used in opto-electronics. Low-temperature solution based methods are of particular interest as possible routes to the low-cost growth of high surface-area nanostructures for the integration of ZnO into novel energy production and storage devices. The steadily growing research areas of solar water splitting and photo-catalysis are prominent examples of areas where interest in ZnO-based materials and devices may be found. [4][5][6][7][8][9][10][11] For these applications the nature of the semiconductor/electrolyte interface plays a crucial role. It is of the highest importance to carefully engineer the materials properties in order ensure effective charge carrier transport across the interface. In turn it must be the goal of materials research to tailor the ZnO toward these target applications, where possible addressing the key issues of:Low visible-light absorption.-Since ZnO exhibits a large bandgap (ca. 3.3 eV) only a small fraction of sunlight is absorbed thus dramatically hindering the use of ZnO for photo-(electro)chemical applications. A common strategy to change the electronic structure of a semiconductor is the introduction of dopants into the host material. In the case of ZnO the material has been doped with various elements whereby many studies focus on doping with transition metals (TMs) such as nickel, magnesium, iron or cobalt.7,12-17 Historically, research focused on transition metal doping has been fueled by the possible creation of ferromagnetism in these materials -especially in the case of cobalt doping. 12,15,[18][19][20][21] On the other h...