We report on optimized wet chemical processes for both the O-polar and Zn-polar faces of wurtzite bulk ZnO single crystals. Different solutions were tested to achieve controllable etching. For the O-polar ZnO surface, a controlled etch rate of 3.8 m/min was observed using an acid mixture of H 3 PO 4 /CH 3 COOH/H 2 O as an etchant. Fine-patterning of the O-polar surface with moderate etch rates and high reproducibility can be obtained using an aqueous 5% NH 4 Cl solution. In comparison, the Zn-polar ZnO surface etches significantly slower in HCl solution and exhibits strong pH dependence. Nevertheless, pH control enables reproducible etching even of the Zn-polar surface.Zinc oxide ͑ZnO͒, one of the most widely investigated wurtzite semiconductors, has attracted significant attention in the past, 1-4 not only as a single crystal but also in the form of polycrystalline thin films. Its remarkable properties, such as its wide direct bandgap ͑3.37 eV͒, large bonding strength ͑cohesive energy of 1.89 eV and melting point of 2248 K͒, and high excitonic binding energy ͑60 meV͒ leading to efficient excitonic optical transitions even at elevated temperatures, make it attractive for electronic and optoelectronic applications such as piezoelectric transducers, transparent thin film electronics, light emitting, and light detecting devices operated in the blue and the ultraviolet spectral range. 5-8 Additionally, ZnO has also found promising applications for nanostructured gas and in chemical and biological sensors. 9 The fabrication of such devices demands the development of etching processes with a controlled degree of anisotropy, with either high or moderate etch rates, and controlled surface morphology for mass production and device reliability. However, wurtzite-type ZnO single crystals exhibit two polar surfaces that are terminated by Znions on the ͑0001͒ plane and O-ions on the ͑0001͒ plane with different chemical and physical properties. 10,11 Therefore, a clear understanding of the chemical reactions during the etch process on each polar face is essential for device patterning. In principle, two methods for planar device patterning have been reported: one method is dry etching such as reactive ion etching using radio frequency or an inductively coupled plasma to remove material from the surface. 12 This method has the benefit of exhibiting the same reaction rates regardless of the crystal orientation. However, it requires expensive investments in equipment. Another method is to use wet chemical etching ͑WCE͒ using liquids, such as the aqueous solutions of acids or mixed acids as etching agents. Compared with dry etch processes, wet etch techniques possess the advantages of simplicity and low equipment cost. Moreover, during dry etching, a hard mask layer such as a metal, SiO 2 , or Si 3 N 4 must often be used as an etch mask because photoresist ͑PR͒ is decomposed under the influence of the plasma, producing carbon residues. This hard mask layer, however, is difficult to remove without attacking the ZnO, depending on it...