Laser cleaning technology, which is environment-friendly, has a wide range of application prospects in remanufacturing, micro-mechanical system (MEMS) and ultra-precision machining. Laser paint removing of aircraft surface is one of the important branches of the technology of laser cleaning. A high repetition frequency CO2 laser, with 10.6 μm wavelength, was used to remove paint, which was double composite paint layer with thickness of 90 μm, from aircraft surface (LY12 aluminum plate). It is shown that totally removed paint stripping and undamaged surface can be reached with selecting appropriate laser power density, scanning distance, and scanning time, the double composite paint layer on aircraft surface can be removed totally, the effect of paint removing on the tensile strength, yield strength, Vickers hardness and roughness of the substrate is studied by the method of experimental contrast. It is found that the mechanical properties of the aircraft surface did not change after the treatment of laser paint removing. Aircraft laser paint removing has more predominance than traditional methods, such as environmental protection without contact, high efficiency, parameters controlling, and low maintenance cost and so on, it develops new directions for applications in other fields.