Currently, biomass transformation to produce high value-added chemicals and liquid biofuels is attracting more and more interest by the virtue of its importance in the sustainable development of human society. Herein, we reported the conversion of furfural (FFA) into cyclopentanone (CPO) in water over high performing and stable Cu/ZrO2 catalysts prepared by our developed one-pot reduction-oxidation method. It was demonstrated that surface structures and catalytic performances of catalysts could be delicately adjusted by varying the calcination temperatures for catalyst precursors. Especially, an appropriate calcination temperature of 500 degrees C could significantly enhance the interactions between surface Cu species and the ZrO2 support, thus greatly facilitating the formation of Cu+-O-Zr-like structure at the metal-support interface, and the resulting Cu/ZrO2 catalyst showed a superior catalytic performance with a high CPO yield of 91.3% under mild reaction conditions (i.e. a low hydrogen pressure of 1.5 MPa and 150 degrees C) to other metal oxides supported copper catalysts prepared by the conventional impregnation. It was revealed that in addition to surface acidic sites, surface Cu+/(Cu degrees + Cu+) ratio also played a key role in promoting the formation of CPO in the present Cu/ZrO2 catalytic system.