<p>A series of NiFex/CeO₂ bimetallic catalysts was prepared by the incipient wetness impregnation method and subsequently applied for CO₂ methanation. The CO₂ methanation activity of the NiFex/CeO₂ catalyst is significantly enhanced by the introduction of an appropriate amount of Fe. At 280&#xa0;°C, 100&#xa0;kPa and 24,000 mL/(g·h), the NiFe0.3/CeO₂ catalyst exhibits a CO₂ conversion of 88.6%. Characterization of the catalysts was performed by N₂ adsorption-desorption, XRD, CO₂-TPD, H₂-TPR and XPS techniques. The results indicate that the introduction of Fe promotes the reducibility of NiO in the catalyst but decreases the number of surface basic sites. A strong electronic interaction between Fe and Ni is observed: Fe³⁺ donates electrons to Ni²⁺ in the calcined catalyst, while after reduction, the formation of a Ni-Fe alloy leads to electron donation from Ni to Fe. The improved catalytic activity of the NiFex/CeO₂ catalysts is attributed to the electronic interaction between Fe and Ni, which modifies the charge density of Ni and enhances the intrinsic activity of Ni sites.</p> Graphical Abstract <p></p> <p>High CO₂ methanation activity was achieved over NiFex/CeO₂ bimetallic catalyst, in which a strong electronic interaction exists between Fe and Ni. </p>