There is provided a coating solution composition of a photo-alignment material. The coating solution composition of the photo-alignment material, adaptive for a photo-alignment process, employs a imidazolidinone-based solvent instead of a typical NMP-based solvent. In a coating method, the photo-alignment material is coated on a substrate in a state that its structure is stabilized in the coating solution through optimization of the coating solution composition. Accordingly, the photoreaction yield increases and a reaction product is stabilized so that a twist angle and a pretilt angle can be improved.