We investigated a solution-derived Y2O3 film treated by ion beam (IB) irradiation as a liquid crystal (LC) alignment layer. With IB irradiation, homogeneous LC alignment was achieved irrespective of the annealing temperature. To verify the effect of IB irradiation, we conducted surface analyses such as X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). As Y2O3 is a high-k material, the electro-optical properties of the twisted nematic (TN) cells were superior to those of conventional TN cells based on a rubbed polymer, with an LC rising time of 4.1ms and falling time of 2.9ms. The IB-irradiated Y2O3 is a good alternative as an alignment layer for fast-switching TN LC displays.