The invention relates to preparation method and device thereof of a surface structuration composite coating, belonging to a film coating of surface engineering. The special device for the preparation method of the surface structuration composite coating is an ultraviolet pulse laser multifunctional surface treatment system device which comprises a pulse laser module, a precise scanning module and an environment regulating module, wherein the pulse laser module, the precise scanning module and the environment regulating module are sequentially connected. The preparation method comprises the steps of primary preparation, surface structuration processing, composite coating deposition and aftertreatment. The invention has novel concept, convenient machining, high efficiency, simple process, easy control and wide application range, the surface structuration treatment of a material and the deposition of the composite coating can be simultaneously realized by adopting a laser light source, surface structuration treatment can be precisely carried on any material, chemical reaction of multiple gases can be induced, and the deposition of the composite coating can be effectively carried out.