A method of fabricating a color filter substrate of an LCD is disclosed. By forming the color filter layer from a hydrophobic material, a fluid black matrix material deposited on the surface of the substrate including the color filter layer flows from the surface of the color filter layer and accumulates between sub-color filters of the color filter layer. The black matrix material is then hardened, permitting the black matrix to be formed between the sub-color filters but not on the color filter layer. Accordingly, the number of mask processes for forming a black matrix is reduced. Further, since the black matrix is only disposed between the sub-color filters, an overcoat layer to eliminate the step difference due to the color filters need not be formed.