With fossil fuels still predicted to contribute close to 80 % of the primary energy consumption by 2040, methods to limit further CO2 emissions in the atmosphere are urgently needed to avoid the catastrophic scenarios associated with global warming. In parallel with improvements in energy efficiency and CO2 storage, the conversion of CO2 has emerged as a complementary route with significant potential. In this work we present the direct thermo‐catalytic conversion of CO2 to hydrocarbons using a novel iron nanoparticle–carbon nanotube (Fe@CNT) catalyst. We adopted a holistic and systematic approach to CO2 conversion by integrating process optimization—identifying reaction conditions to maximize conversion and selectivity towards long chain hydrocarbons and/or short olefins—with catalyst optimization through the addition of promoters. The result is the production of valuable hydrocarbons in a manner that can approach carbon neutrality under realistic industrial process conditions.