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Abstract: The electrochemical CO2 reduction (ECDRR), as a key reaction in artificial photosynthesis to implement renewable energy conversion/storage, has been inhibited by the low efficiency and high costs of the electrocatalysts. Herein, we synthesize a fluorine‐doped carbon (FC) catalyst by pyrolyzing commercial BP 2000 with a fluorine source, enabling a highly selective CO2‐to‐CO conversion with a maximum Faradaic efficiency of 90 % at a low overpotential of 510 mV and a small Tafel slope of 81 mV dec−1, outcompeting current metal‐free catalysts. Moreover, the higher partial current density of CO and lower partial current density of H2 on FC relative to pristine carbon suggest an enhanced inherent activity towards ECDRR as well as a suppressed hydrogen evolution by fluorine doping. Fluorine doping activates the neighbor carbon atoms and facilitates the stabilization of the key intermediate COOH* on the fluorine‐doped carbon material, which are also blocked for competing hydrogen evolution, resulting in superior CO2‐to‐CO conversion. [ABSTRACT FROM AUTHOR]