We used four saturated fatty acids as the simple alignment agent for orienting liquid crystals (LCs) vertically on an indium tin oxide (ITO) substrate without using a conventional polyimide (PI) layer. The carboxylic acid group of fatty acids doped in LC media forms hydrogen bonds with the ITO substrate, leading to the formation of self-assembled molecular layer containing alkyl chains for LC alignment. The proposed method offered uniform vertical alignment of LCs under cross-polarization. Further, the electro-optical characteristic of the proposed LC device showed better performance than that of the LC cell with conventional PI alignment layer.