High-current pulsed electron beam (HCPEB) technique was applied to irradiate the samples of pure zirconium. The microstructures and defects of the irradiated surface are investigated by using X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). XRD results show that the high value of stress (GPa order) is introduced within the irradiated surface layer, while the formation of {0002}, {1012}, {1120} and {1013} textures are present after HCPEB irradiation. Microstructure observations demonstrate that the surface craters are rarer, and almost no craters are present after multiple pulses HCPEB irradiation, which is evidently different from the case of other metal materials irradiated by HCPEB. Moreover, a large number of ultrafine grains are formed on the irradiated surface. Martensitic transformation occurs and severe plastic deformation is also induced due to the superfast melting and cooling processes. After one- pulse irradiation, the dislocations are the dominant defects, while the amount of twins is less. After five pulses, the dislocation density and the number of deformation twins increase evidently, whereas dense deformation twins are the central microstructures after ten-pulse irradiation, coupled with the appearance of secondary twins occasionally. The formation of these deformed structures results in a significant effect both on the evolution of surface textures and on grain refinement. It is suggested that HCPEB technique provides an impactful approach for hardening of zirconium and zirconium alloys.