A cubic fluorite-type CeO 2 with mesoporous multilayered morphology was synthesized by the solvothermal method followed by calcination in air, and its oxygen storage capacity (OSC) was quantified by the amount of O 2 consumption per gram of CeO 2 based on hydrogen temperature programmed reduction (H 2 -TPR) measurements. Doping CeO 2 with ytterbium (Yb) and nitrogen (N) ions proved to be an effective route to improving its OSC in this work. The OSC of undoped CeO 2 was 0.115 mmol O 2 /g and reached as high as 0.222 mmol O 2 /g upon the addition of 5 mol.% Yb(NO 3 ) 3 ∙5H 2 O, further enhanced to 0.274 mmol O 2 /g with the introduction of 20 mol.% triethanolamine. Both the introductions of Yb cations and N anions into the CeO 2 lattice were conducive to the formation of more non-stoichiometric oxygen vacancy ( V O ) defects and reducible-reoxidizable Ce n+ ions. To determine the structure performance relationships, the partial least squares method was employed to construct two linear functions for the doping level vs. lattice parameter and [ V O ] vs. OSC/ S BET .