Lasers and electron beams have been widely used to synthesize various surface alloys (SAs) but no data have been reported so far on the molybdenum-zirconium (Mo-Zr) ones. To partially fill this knowledge gap, Mo-Zr SAs were formed by processing molybdenum films on zirconium substrates with low-energy high-current electron beams (LEHCEBs). The effect of the energy density of LEHCEBs on the microstructure, phase composition, nanohardness and corrosion resistance of the Mo-Zr SAs were investigated. Basically, the Mo-Zr SAs consisted of a solid solution of Mo in the β-Zr phase, Mo2Zr second phase particles (SPPs) and a solid solution Zr in Mo. Increasing in the energy density decreased the concentration of the SPPs and enhanced the content of the β-Zr phase. Also, it affected the depth of the highest concentration of the SPPs. In the zones of the highest molybdenum contents, the nanohardness values reached 9.4–12.7 GPa, which was higher by 3.2–4.4 times than that of the zirconium substrates. In a 3.5 % NaCl solution at room temperature, the corrosion current densities and the corrosion potentials were greater than those of the zirconium substrates by six and almost two times, respectively.