In space optical communications, it is important to obtain the most efficient performance of line of sight (LOS) pointing system. The errors of position (latitude, longitude, and altitude), attitude angles (pitch, yaw, and roll), and installation angle among a different coordinates system are usually ineluctable when assembling and running an aircraft optical communication terminal. These errors would lead to pointing errors and make it difficult for the LOS system to point to its terminal to establish a communication link. The LOS pointing technology of an aircraft optical communication system has been researched using a transformation matrix between the coordinate systems of two aircraft terminals. A method of LOS calibration has been proposed to reduce the pointing error. In a flight test, a successful 144-km link was established between two aircrafts. The position and attitude angles of the aircraft have been obtained to calculate the pointing angle in azimuth and elevation provided by using a double-antenna GPS/INS system. The size of the field of uncertainty (FOU) and the pointing accuracy are analyzed based on error theory, and it has been also measured using an observation camera installed next to the optical LOS. Our results show that the FOU of aircraft optical communications is 10 mrad without a filter, which is the foundation to acquisition strategy and scanning time.