The results of experimental studies on the modification of the surface layer of zirconium alloy grade E 110 by the action of pulsed laser radiation are presented. It was established that, as a result of laser treatment, the morphology of the surface layer changes with the formation of nanoparticles up to 50 nm in size. The relief of the treated surface becomes structurally heterogeneous, containing phases of zirconium and monoclinic ZrO2 dioxide. It was revealed that, as a result of exposure to laser pulses, a significant increase in the microhardness of the surface of zirconium samples occurs to 27.1 ± 0.1 GPa.