In order to improve the wear and corrosion resistance and enhance the tribological and mechanical properties of gray cast iron, the laser surface cladding technique was employed to fabricate double-layer coatings with different Ni/WC ratios on the surface of gray cast iron. The effects of laser processing parameters and the type of Ni-based alloy on the microstructure and properties of the gray cast iron matrix and laser-clad layer were investigated. A 316L stainless steel transition layer was introduced between the gray cast iron substrate and the Ni/WC coating to prevent the cladding layer from cracking. The tribological and mechanical properties of the laser-clad coatings were characterized with various tests at the macro- and micro-scales; the residual stresses on the coating surfaces were measured, and electrochemical tests were also carried out. The microstructures of the clad layers were analyzed by scanning electron microscope (SEM) and X-ray diffraction (XRD). The results show that the laser-clad layers exhibit excellent vibration and noise reduction performance, which is partially due to the reduction and stabilization of the coefficients of friction (COFs) and the high levels of compressive residual stress on the surface of the laser-clad layers. The wear and corrosion resistance of the laser-clad layers are significantly improved, and the maximum wear loss of the laser-clad coating was about only 5% of that of the unclad gray cast iron substrate. This research has significance for the laser surface modification of cast iron, steel, and other metals, which is an increasingly important topic, especially in the automotive friction brake industry.