A method of manufacturing an alignment film is provided, and has steps of determining printing regions for an alignment agent, which including display portions and transfer portions; printing the alignment agent within the printing regions to form an alignment thin layer; and performing an alignment process to the alignment thin layer to form the alignment film. The unevenness on the edge of the alignment film is moved away from the display portions by expanding the printing regions for the alignment agent, so as to promote the imaging quality of the finished LCD.