Laser peen forming (LPF) is a purely mechanical forming method achieved through the use of laser energy to form complex shapes or to modify curvatures. It is flexible and independent of tool inaccuracies that result from wear and deflection. Its nonthermal process makes it possible to form without material degradation or even improve them by inducing compressive stress over the target surface. In the present study, a fully three-dimensional numerical model is developed to simulate the forming process of laser peen forming. The simulation procedure is composed of several steps mainly including the shock pressure prediction, the modal analysis, and the forming process calculation. System critical damping is introduced to prevent unnecessary long post-shock residual oscillations and to greatly decrease the solution time for simulation. The bending profiles and angles with different thicknesses are experimentally measured at different scanning lines and scanning velocities to understand the process and validate the numerical model. The calculated bending profiles and angles agree well with the trend of the measured results. But it is found that simulations with the Johnson–Cook model are more consistent, matching the experimental results for the thick sheet metal with a convex bending, while the elastic-perfectly-plastic model produces a better agreement even though with underestimated values for the thinner sheet metal with a concave bending. The reason for this phenomenon is discussed, combining the effects of strain rate and feature size. Both the simulation and the experiments show that a continuous decrease in bending angle from concave to convex is observed with increasing specimen thickness in general. Large bending distortion is easier to induce by generating a concave curvature with LPF, and the angle of bending distortion depends on the number of laser shocks.