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Greenhouse effects and global warming mainly result from the CO2 generation by rapid industrialization and economic development. Exploitation of highly efficient and robust carbon-based adsorbents benefits the reduction of CO2. In this review, several representative carbonaceous materials (e.g., activated carbons, coal-derived carbons, polymer-derived carbons, metal-organic frameworks-derived carbons, carbon nanotubes, graphene oxides and carbon aerogels) as CO2 adsorbents are discussed comprehensively, including the carbonization (e.g., pyrolysis, hydrothermal treatment), activation (e.g., physical and chemical treatment) and modification (e.g., doping and heterostructure) process. The synthesis-structure-performance relationships are elucidated in depth. Finally, the conclusive remarks and future works are also proposed.