Laser cleaning is an efficient, environmental-friendly, and non-contact surface treatment technology. Laser radiation and heating cause the surface material to heat up and gasify, separating it from the substrate. Traditional mesh-based numerical methods are difficult to effectively simulate the evolution of erosion crater and the splashing phenomenon. In this study, a meshfree method, the smoothed particle hydrodynamics (SPH) method, is used to establish the numerical model of the interaction between the laser beam and the targeted material and to investigate the removal process of the rust layer under different laser operating conditions. In consideration of the coupling effect of laser absorption, heat transfer, and material phase change, the SPH modeling procedure and corresponding numerical scheme for heat transfer and heat-absorption-induced phase change are introduced. Additionally, a surface particle detection algorithm and surface normal vector calculation method are proposed to accurately compute the complex surface geometry of the erosion crater, which realizes the dynamic coupling of laser-energy absorption and laser-beam direction. The established SPH model is then used to simulate the temperature distribution of the rust layer under the action of a laser beam, and the influence of laser energy, beam overlap rate, and beam direction on the removal efficiency is analyzed. This study applies the meshfree SPH method to the study of laser rust removal process, verifies the accuracy of the surface detection algorithm, captures the spatter behavior of material particles after phase change, and reflects the advantages of the meshfree method in solving such problems.