ZnO nanosheets have been used for many devices and antibacterial materials with wide bandgap and high crystallinity. Among the many methods for synthesizing ZnO nanostructures, we report the synthesis of ZnO/Zn(OH)2 nanosheets using the ionic layer epitaxy method, which is a newly-developed bottom-up technique that allows the shape and thickness of ZnO/Zn(OH)2 nanosheets to be controlled by temperature and time of synthesis. Results were analyzed by scanning electron microscopy and atomic force microscopy. The physical and chemical information and structural characteristics of ZnO/ Zn(OH)2 nanosheets were compared by X-ray photoelectron spectroscopy and X-ray diffraction patterns after various posttreatment processes. The crystallinity of the ZnO/Zn(OH)2 nanosheets was confirmed using scanning transmission electron microscopy. This study presents details of the control of the size and thickness of synthesized ZnO/Zn(OH)2 nanosheets with atomic layers.