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Fossil fuel carbon dioxide (FFCO₂) is a major source of atmospheric greenhouse gases that result in global climate change. Quantification of the atmospheric concentrations and emissions of FFCO₂ is of vital importance to understand its environmental process and to formulate and evaluate the efficiency of carbon emission reduction strategies. Focusing on this topic, we summarized the state-of-the-art method to trace FFCO₂ using radiocarbon (¹⁴C), and reviewed the ¹⁴CO₂ measurements and the calculated FFCO₂ concentrations conducted in the last two decades. With the mapped-out spatial distribution of ¹⁴CO₂ values, the typical regional distribution patterns and their driving factors are discussed. The global distribution of FFCO₂ concentrations is also presented, and the datasets are far fewer than ¹⁴CO₂ measurements. With the combination of ¹⁴C measurements and atmospheric transport models, the FFCO₂ concentration and its cross-regional transport can be well interpreted. Recent progress in inverse methods can further constrain emission inventories well, providing an independent verification method for emission control strategies. This article reviewed the latest developments in the estimation of FFCO₂ and discussed the urgent requirements for the control of FFCO₂ according to the current situation of climate change.