The invention relates to the field of laser processing, in particular to a method and a device for compositely preparing a surface-layer biomimetic structure by mechanical effects based on laser carving and laser shock, which are particularly suitable for processing a biomimetic surface and a friction pair surface. The method is characterized by comprising the following steps: firstly preparing aregular micro geometrical appearance with certain density (space), width, depth, angle and shape on the surface of a workpiece by the laser carving technology; and then forcedly processing the micro geometrical appearance area by laser shock to process a microstructure which has the required shape and management mode and is optimally matched with the requirement of lubricating property on the surface of the workpiece. The device for the implementation method comprises a control device, a nanosecond laser generator, a laser beam I, a light guide tube I, a totally reflecting mirror I, a light spot adjusting device I, a fiber laser, a laser beam II, a light guide tube II, a totally reflecting mirror II, a light spot adjusting device II, an automatic spraying device, a restrain layer, an absorption layer, the workpiece, a workpiece fixture system and a five-axis working platform.