The CrMnFeCoNi alloy with a stable single face-centered cubic (FCC) phase, representing a typical class of high-entropy alloys (HEAs), has garnered considerable attention owing to their exceptional mechanical properties. However, the inherent low hardness has impeded their utilization in structural or contact components. This study attempted to improve the surface hardness of CrMnFeCoNi HEA via grain refinement realized by nanosecond pulse laser irradiation. The effects of laser parameters on the surface microstructures, chemical composition, and mechanical properties were investigated, and the mechanism for grain refinement was analyzed. The experimental results showed that the hardness of the laser-irradiated surface was significantly improved without altering the chemical composition. This study provides a simple but effective method to refine the grain of HEAs and improve their surface hardness. •Grain refinement was achieved on CrMnFeCoNi HEA via nanosecond laser irradiation.•Surface hardness of the irradiated surface was significantly improved.•The effect of laser parameters on microstructures and hardness was investigated.