A variety of CeO2-Al2O3 composite oxides were prepared using a citric acid complexation method by varying the amount of CeO2 in the material from 5 to 30 wt.%. Using these as-prepared composite oxides as the supports, a series of Pd/CeO2-Al2O3 catalysts with 5 wt.% of Pd loading were prepared by a deposition-precipitation method. The physico-chemical properties of the catalysts were characterized by XRD, N2 adsorption-desorption, TEM and XPS technologies. Moreover, the performance of the catalysts was investigated for the one-pot reductive amination of levulinic acid with nitriles and H2 towards N-substituted 5-methyl-2-pyrrolidones. The results showed that the Pd/10%CeO2-Al2O3 catalyst exhibited the best performance, over which an 87.5% yield of N-benzyl-5-methyl-2-pyrrolidone was achieved through the reductive amination of levulinic acid with benzonitrile under mild reaction conditions (90?C, 1.5 MPa H2) for 5 h. Meanwhile, Pd/10%CeO2-Al2O3 was efficient for the reductive amination of levulinic acid/ester with various nitriles to give high yields of pyrrolidones (76.3%-87.4%). The catalyst was reused for 5 times, and its activity did not decrease significantly.