Ni-loaded CeO 2 -based materials are one type of the promising catalyst for CO 2 methanation; however, lowering the Ni loading, simplifying the preparation process of CeO 2 supports, and improving the low-temperature catalytic performance are always essential for scalable applications. Herein, an efficient CeO 2 support (CeO 2 -NC) with a large inner pore size was prepared by a facilely controlled calcination of cerium nitrate [Ce(NO 3 ) 3 •6H 2 O] method. On the basis of CeO 2 -NC, one catalyst (Ni/CeO 2 -NC) with low Ni loading (2.56 wt %), desirable Ni dispersity, and abundant medium basic sites was developed that exhibited the amazing low-temperature CO 2 methanation performance. At 275 °C, CO 2 conversion reached up to 77.7% with an almost 100% CH 4 selectivity under a high gas hourly space velocity of 60000 mL g cat −1 h −1 , and the Ni-based mass-specific CH 4 formation rate at 300 °C was up to 4740 μmol g Ni −1 s −1 , outperforming most of the reported Ni-based catalysts to date. The in situ diffuse-reflectance infrared Fourier transform spectroscopy experiments revealed that plentiful active bidentate carbonate intermediates and effective suppression of the dissociated active H species recombination contributed to the boosted CO 2 methanation performance of Ni/CeO 2 -NC at low temperatures. Moreover, the mechanism was also inferred. This work provides new insight into simple pyrolysis CeO 2 supports and should be of significance for the rational design of highly efficient CO 2 methanation catalysts.