A combined method of modified oblique-angle deposition and hydrothermal growth was adopted to grow an optically anisotropic nanomaterial based on single crystalline ZnO nanowire arrays (NWAs) with highly oblique angles (75°-85°), exhibiting giant in-plane birefringence and optical polarization degree in emission. The in-plane birefringence of oblique-aligned ZnO NWAs is almost one order of magnitude higher than that of natural quartz. The strong optical anisotropy in emission due to the optical confinement was observed. The oblique-aligned NWAs not only allow important technological applications in passive photonic components but also benefit the development of the optoelectronic devices in polarized light sensing and emission.