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Hydrogenation of CO 2 to olefin catalyzed by iron-based catalysts is a sustainable and important way to achieve carbon neutrality. In this study, iron-based catalysts were facilely prepared by direct pyrolysis of ferric fumarate (FF), which are applied to CO 2 hydrogenation to olefin reaction to explore the effects of pyrolysis temperature and atmosphere on catalytic performance of the catalysts. Among them, NaFe-Air-400 catalyst exhibits the highest catalytic activity with 33.7 %, and light olefin selectivity reaches as high as 47.1 %. The catalytic performance of pyrolytic catalysts is better than that the impregnated NaFe catalyst on activated carbon (NaFe/AC). A series of XRD, Raman and SEM characterization results show a suitable pyrolysis temperature would promote the balance between amorphous carbon and graphene, which can affect the formation of Fe x C y phase, leading the distinctive activity and olefin selectivity. Hence, the presented one-step pyrolysis methodology would provide a facile and quick synthesis of highly-active iron-based catalyst design for CO 2 conversion., (© 2024 Wiley‐VCH GmbH.)