CoFe2O4 nanoparticles were synthesized as efficient catalyst precursors for CO2 hydrogenation to produce C2–C4 olefins. The resulting Na–CoFe2O4 catalyst exhibits high CO2 conversion (~34%) and light olefin selectivity (~39%). The excellent performance of the Na-CoFe2O4/CNT catalyst can be attributed to unique bimetallic alloy carbide (Fe1-xCox)5C2.