In this paper, we discuss double-pulse laser peening (DPLP) as surface enhancement technology. Although single-pulse laser peening (SPLP) has yielded excellent results across various applications, its processing performance and efficiency are limited. The DPLP technique involves two laser pulses with a controlled irradiation interval and intensity, enhancing laser absorption through the plasma plume and generating high-amplitude laser-induced shock waves. This study involved conducting DPLP experiments on stainless steel, comparing the outcomes with those of conventional SPLP to assess DPLP’s functionality. After the initial prepulse irradiation, the subsequent main pulse was timed and irradiated onto the stainless steel. We evaluated the surface hardness to ascertain the impact of laser peening. The findings indicated that the surface hardness achieved with DPLP was up to 64% greater than that with SPLP. Additionally, the surface hardness achieved through DPLP depended on the delay time between the pulses and the intensity of the initial prepulse. These findings suggest that DPLP can significantly enhance surface hardness, providing a potential pathway for improving material performance in various industrial applications. Furthermore, simulation experiments of DPLP were performed using a one-dimensional simulation code that calculates the laser-matter interaction during the peening process. The pressure profiles generated by the simulation closely matched the experimentally derived hardness profiles, confirming the simulation’s ability to predict the mechanical effects induced by DPLP on the target sample and assist in further optimization of the DPLP process.