Abstract The quantitative relationship between nanosecond pulsed laser parameters and the characteristics of laser-generated ultrasonic waves in polycrystalline materials was evaluated. The high energy of the pulsed laser with a large irradiation spot simultaneously generated ultrasonic longitudinal and shear waves at the epicenter under the slight ablation regime. An optimized denoising technique based on wavelet thresholding and variational mode decomposition was applied to reduce noise in shear waves with a low signal-to-noise ratio. An approach for characterizing grain size was proposed using spectral center frequency ratio (SCFR) based on time-frequency analysis. The results have demonstrated that the generation regime of ultrasonic waves is not solely determined by the laser power density; even at high power densities, a high energy with a large spot can generate an ultrasonic waveform dominated by the thermoelastic effect. It is ascribed to the intensification of the thermoelastic effect with the proportional increase in laser irradiation spot area for a given laser power density. Furthermore, both longitudinal and shear wave SCFRs are linearly related to grain size in polycrystalline materials; however, the shear wave SCFR is more sensitive to finer-grained materials. This study holds great significance for evaluating metal material properties using laser ultrasound.