This study led to the development of a fast switching liquid crystal (LC) device based on a self-assembled molecular layer of bifunctional reactive amphiphiles. The bifunctional reactive amphiphile was designed to contain a carboxylic acid group capable of undergoing hydrogen bonding with the indium-tin-oxide substrate and a photoreactive functional group to accomplish pre-tilt of the LCs at the other end. The unique structural arrangement of the reactive amphiphiles with their two side arms ensures that the LC molecules are vertically oriented without the aid of polyimide, and fast response can be realized by implementing pre-tilt formation by using UV photopolymerization.