Laser surface modification is a widely used technology to improve the properties of functional surfaces. In this study, the properties of gray cast iron are modified by laser surface modification, and the influence of laser quenching on the properties of cast iron in terms of frictional vibration and noise, friction and wear, internal structure, residual stress, hardness, and corrosion resistance is investigated. The experimental results show that, after high-power laser quenching, the frictional vibrations and noise of most gray cast iron specimens are decreased, but the coefficients of friction against a bearing steel counterface are increased and more stable. The surface and sub-surface hardness of all laser-quenched cast iron specimens is significantly increased. The residual stresses on the surface of the cast iron specimens are significantly increased and changed from tensile to compressive residual stresses. Experimental modal testing results show that the modal damping ratios of the laser-treated specimens are increased significantly, although their modal frequencies are not significantly changed. In addition, through the metallographic observation, XRD (X-ray diffraction) analysis, and TEM (transmission electron microscopy) observation, it is found that the microstructures of the cast iron specimen after high-power laser modification become fine-grained, and the pearlite and ferrite in the matrix become fine martensite, which leads to the improvement of the dynamical, tribological, and chemical properties of cast iron after laser modification.