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The “HOPE-I” type high-current pulsed electron beam (HCPEB) equipment was used to irradiate the pure aluminum material with Zr coating preset by ball milling to realize the alloying of a Zr–Al coating surface. The microstructure and phase analysis were conducted by XRD, SEM, and TEM. The experimental results show that after Zr alloying on the Al surface by HCPEB, a layer of 15 μm was formed on the surface of the sample, which was mainly composed of Zr and Al–Zr intermetallic compounds. A large number of Al3Zr (Ll2) particles was uniformly distributed in the alloyed layer, and the Al grains were obviously refined. In addition, the surface hardness and corrosion resistance of the samples were improved significantly after HCPEB irradiation.