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Nanostructured Cobalt‐Actinide (An=Th, U) bimetallic oxides were for the first time prepared by the epoxide addition method and electrospinning technique aiming the synthesis of aerogels and nanofibers, respectively. Tested as catalysts for the methanation of CO2 and regardless of the actinide element, the yield and selectivity towards CH4 are high (>40 and 95 %, respectively), which was explained by their physicochemical properties such as reducibility and basicity and the existence of a synergic effect between cobalt and actinide species. The aerogels present the best catalytic behavior, namely those with thorium and the catalytic activity increases with the Co/An molar ratio. Both aerogels and nanofibers also present a high resistance to deactivation for at least 75 h in the gaseous stream, which is an advantage for any catalytic application. Moreover, at 300 °C they are 2 to 4 times more active than two reference catalysts (5wt % Rh/Al2O3 and NiO/Al2O3) tested in the same conditions, which to our best knowledge is a significant result. [ABSTRACT FROM AUTHOR]