The laser shocks of different pulse energies are used to perform a single impact on every multi-point of three kinds of the film-substrate system with different interface bonding strengths. The residual stress of target surface is detected by X-ray diffraction (XRD) technique, and the dynamic strain signal is collected by polyvinylidene fluoride (PVDF) sensor. Then a loading model of the laser shock wave on film-substrate system is established. Finally, the failure modes of film-substrate system based on laser discrete scratch are explored. The results show that the residual stress both on the surface of the 2024 aluminum alloy and the impact spot center of the film-substrate system increase after laser shock. The dynamic response of film-substrate system is related to the bond strength of film-substrate interface and the energy of laser. There are two failure modes of film-substrate system based on laser discrete scratch, one is the reflect stretch wave lead to membrane detached from the substrate, the other one is the shear stress of film-substrate system lead to film shear failure.