We demonstrated homogeneous liquid crystal (LC) alignment on Nickel Oxide (NiO) films subjected to ion beam (IB) irradiation. Uniform LC alignment was achieved at high IB intensity values of 1200 and 1800 eV. To determine the mechanism of LC alignment following IB irradiation, physicochemical analysis was performed using atomic force microscopy and X-ray photoelectron spectroscopy. IB irradiation with high intensity increases uniformity of the surface, and IB irradiation induces the formation of oxygen vacancies and increases the NiO (Ni2+) phase components. Hence, both of the smooth surface and the strong van der Waals interactions between the NiO film and the LC molecules provides the LC molecules with a stable anchor on the surface, leading to uniform LC alignment on NiO films after IB irradiation. IB-irradiated NiO exhibited a high transparency of 85% in the visible light range as compared with the 83% average transmittance of conventional polyimide, which makes the IB-irradiated NiO alignment layer attractive in display devices.