In modern combat, laser weapons are widely used due to their high precision, velocity and heat detriment. Hence, it is of great importance to fabricate protective coating on the surface of core components, i.e. gasoline tank and aerofoil. In this study, an organosilicone composite coating was prepared on steel and aluminum substrates through a simple spray process to resist laser ablation destroy. This composite coating consists of organic resin base and inorganic functional fillings, which were made up of glass powder with high melting point materials such as SiO2, BN and ZrO2 etc. Laser ablation resistance behavior was studied by means of oxyacetylene torch and laser irradiation. Results demonstrate that the coating presents excellent heat resistant behavior under 3000°C. Moreover, after impulse laser attack up to 105W/cm2, both substrates remain unhurt. As a result, this organosilicone composite coating can be used for anti-laser application in various fields.