The hydrogenation of benzene over amorphous Ni-Zr alloys with different Ni compositions (Ni33Zr67, Ni40Zr60, Ni50Zr50, Ni70Zr30, Ni90Zr10) produced by means of a rapid solidification technique was investigated. Although the catalytic activities of the alloys were very low in the virgin state, they gradually increased with increasing number of regeneration (oxidation and reduction) reaction cycles, and the activity approached a constant value after six regenerations. The benzene hydrogenation activity increased with nickel content up to 50%, but then decreased with Ni content. It was shown that the surface area measured by the nitrogen adsorption method had almost the same dependence on Ni content. These results suggest that the Ni50Zr50 alloy is easily relaxed by the regeneration, and Ni atoms effective for the hydrogenation are highly dispersed on the micro ZrO2 crystals produced from the alloy by the oxidation.