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Copper doped ceria porous nanostructures with a tunable BET surface area were prepared using an efficient and general metal-organic-framework-driven, self-template route. The XRD, SEM and TEM results indicate that Cu 2+ was successfully substituted into the CeO 2 lattice and well dispersed in the CeO 2 :Cu 2+ nanocrystals. The CeO 2 :Cu 2+ nanocrystals exhibit a superior bifunctional catalytic performance for CO oxidation and selective catalytic reduction of NO. Interestingly, CO oxidation reactivity over the CeO 2 :Cu 2+ nanocrystals was found to be dependent on the Cu 2+ dopants and BET surface area. By tuning the content of Cu 2+ and BET surface area through choosing different organic ligands, the 100% conversion temperature of CO over CeO 2 :Cu 2+ nanocrystals obtained from thermolysis of CeCu-BPDC nanocrystals can be decreased to 110 °C. The porous nanomaterials show a high CO conversion rate without any loss in activity even after five cycles. Furthermore, the activity of the catalysts for NO reduction increased with the increase of BET surface, which is in accordance with the results of CO oxidation.