The effect of laser irradiation with different numbers of laser shots on the microstructure, the surface, and the hardness of gun metal alloy was studied by a KrF pulsed excimer laser system, X-ray diffraction, Raman spectroscopy, scanning electron microscopy, and Vickers hardness test. The influence of 100–500 laser shots was irradiated on the surface hardness profile and on the microstructure of gunmetal alloy. XRD results showed the maximum 2θ shift, the maximum full width of half maximum FWHM, the maximum dislocation density, and the minimum crystallite size for the sample irradiated with 300 laser shots. The hardness was measured in three different regions at the laser irradiated spot, and it was found that maximum hardness was present at the heat affected zone for all samples. The hardness value of the un-irradiated sample of gun metal was 180, and the value increased up to 237 by raising the number of laser shots up to 300. The peak value of surface hardness of the laser treated sample was 32% higher than the un-irradiated sample. The Raman shift of the un-exposed sample was 605 cm−1 and shifted to a higher value of wave number at 635 cm−1 at 300 laser shots. The hardness value was decreased by further increasing the number of laser shots up to 500. The samples irradiated with 400 and 500 laser shots exhibited smaller hardness and dislocation defect density, which was assigned to possible annealing caused by irradiation.