Mechanochemical activation, by means of high-energy ball milling, was applied to CeO2 as a strategy to enhance its physicochemical properties. Different milling parameters such as rotational speed and milling time were screened to evaluate their effect on ceria. Fluorite-type structure of cerianite was maintained in all cases, no matter the amount of energy introduced by milling process, as observed by X-ray Diffraction (XRD). A decrease in crystallite sizes along with a consequent increase in Specific Surface Area (SBET) were observed by XRD and N2 sorption (BET method). Pore diameters and total pore volumes were also in line with the duration of CeO2 milling. Moreover, redox properties and oxygen mobility studied by H2-Temperature Programmed Reduction (H2- TPR) showed an increase in reducibility with milling time, including signals of both bulf and surface ceria, due to the greater number of defects and/or oxygen vacancies achieved by mechanochemical activation. Obtained features could play an essential role in terms of metal-support interaction, reactants adsorption and/or oxygen supply during catalytic reactions. Thus, high-energy ball milling becomes a useful, simple and green method for materials design with catalytic applications.