The nanostructure Ce0.75Zr0.25O2powders have been successfully synthesized by using the mechanically activated solid-state chemical reaction method for the first time, with Ce2(CO)3, ZrOCl2⋅8H2O, and H2C2O4⋅2H2O as raw materials. The structure and morphology of Ce0.75Zr0.25O2powders were characterized to be in the single cubic phase and spherical shape via X-ray powder diffraction, transmission electron microscopy, X-ray Photoelectron Spectrometer, and BET surface area testing technique. The average size of particles was measured to be less than 20 nm, and the specific surface area was 85.4 m2/g. The TG-DTA investigation was used to reveal the possibly chemical reaction mechanism during the synthesis process. The activity of Ce0.75Zr0.25O2oxide solution in three-way catalysts was also valued in this work.