gamma-Valerolactone (GVL) has been identified as a key intermediate for the sustainable production of fuels and value-added chemicals. In this work, an efficient NixZryO catalyst was prepared by co-precipitation and used in the low pressure hydrogenation to prepare GVL from bio-derived methyl levulinate (ML) in aqueous solution. Several catalysts that differed in their Ni/Zr molar ratio were prepared and characterized by BET, XRD, H-2-TPR, NH3-TPD and XPS, and they exhibited different catalytic activities in the catalytic hydrogenation reaction of ML. The best catalytic activity was realized with NilZr10, which gave a 96.9% yield of GVL by low hydrogen pressure at 0.3 MPa in the aqueous solution at 150 degrees C. By comparison with NiO and Raney Ni, it was found that introducing zirconium into nickel oxide remarkably enhanced the performance of the NixZryO catalysts. According to the XRD, H-2-TPR and XPS results, when a certain amount of zirconium was introduced (e.g., Ni/Zr = 1), part of the nickel either coordinated with zirconium or formed NimZrnO quaSi solid solution and was not readily reduced by H-2. Theoretical calculations showed that the formed Ni - O - Zr species was superior to pure nickel or zirconium oxides for the adsorption of ML. The synergy between metallic nickel, which activated H-2, and the Ni - O - Zr species, which activated ML, was believed to expedite the production of gamma-valerolactone. Moreover, NilZr10 showed good catalytic stability and retained the catalytic performance even after five reaction cycles of the ML hydrogenation.