Electrostatic potential barriers at doped ZnO-ZnO interfaces can be modified by stress-induced polarization charges. This concept was enhanced by preparing ZnO-based single crystal-polycrystal-single crystal structures by diffusion bonding. Increasing time for epitaxial solid-state transformation results in structures with a decreasing thickness of residual polycrystalline material in between two well-oriented single crystals. Microstructural and electrical analysis quantifies the influence of high-temperature treatment during epitaxial growth on the stress sensitivity of the prepared structures. The orientation of the single crystals is defined to maximize the interaction between stress-induced polarization charges and the potential barriers at doped ZnO-ZnO interfaces. With decreasing thickness of residual polycrystalline material, the percentage of grain boundaries with favorably aligned polarization vectors is increased resulting in a higher stress sensitivity. This effect is compensated by an adverse effect of the high-temperature treatment on the initial potential barrier height. Hence, a maximum in stress sensitivity can be observed for intermediate times of epitaxial growth. The prepared structures close the gap between the varistor piezotronics based on bulk ceramics with random orientation of the polarization vector and the bicrystal piezotronics with perfect orientation of the polarization vector, demonstrating the capability of microstructural engineering for varistor-based piezotronic devices.