The structural characteristics of aerial infrared cameras were analyzed, and the key technologies of alignment of this type of cameras were validated. A method for adjustment and validation of a single camera was proposed. The method adjusted the camera coarsely based on measuring the line array direction and optical axis direction of a detector by a theodolite, and adjusted the camera finely by combining with the sub-pixel subdivision location algorithm. A scheme to complete a one-time adjustment by covering all lenses was proposed based on a large diameter parallel light pipe and a high precision controlled turntable, by which the grouped alignment and validation for the aerial infrared camera were implemented. The simulation results show that the method meets the demands of aerial infrared camera for high accuracy alignment and small tolerances. The adjustment precision of the angle among the boresights of multi-angle camera has reached 0.57 pixel, which is about 20 times that of the traditional methods. The proposed method provides a practical and feasible way to adjust precisely aerial infrared cameras and can be used in adjustment for other aerial sensors with similar structures.