We have studied the liquid crystal (LC) orientation behavior on the organic hybrid overcoat layer with ion beam irradiation. Excellent LC alignments of the nematic liquid crystal (NLC) on the ion beam irradiated organic hybrid overcoat layers were observed in various intensities above 600 eV. Pretilt angles of the NLC on the organic hybrid overcoat layers for all ion beam energy intensities were observed from 0.2 to 0.5 degrees. Also, we used the atomic force microscopy (AFM) images for measuring the roughness of the organic hybrid overcoat layers with ion beam irradiation before and after. The surface of organic hybrid overcoat layers was leveled off by the ion beam irradiation. Finally, a good LC alignment thermal stability on the organic hybrid overcoat layer with ion beam irradiation can be achieved.