Solution-derived HfYGaO films have been treated by ion beam (IB) irradiation and used as liquid crystal (LC) alignment layers. Solution processing was adopted due to its simplicity, high throughput, and facile composition modification. Homogeneous and uniform LC alignment was achieved on the IB-irradiated HfYGaO films, and when these films were adopted in twisted nematic (TN) cells, electro-optical performance comparable to that of TN cells with conventional polyimide layers was achieved, with almost no capacitance-voltage hysteresis. Moreover, LC cells based on IB-irradiated HfYGaO films had a high thermal budget. The proposed IB-irradiated solution-derived HfYGaO films have considerable potential for use in advanced LC applications.