Carbon materials have been considered to be one of the most promising candidates for CO2 capture due to their specific features such as low price, high specific surface area, hydrophobic surface, excellent thermal and chemical stability, and low energy requirements for regeneration. This chapter aims to summarize the recent research progress made in developing carbon-based adsorbents for post-combustion CO2 capture. Specifically, this chapter provides overviews of (1) porous carbons, (2) graphene-based porous materials, (3) carbon nanotubes, (4) carbon-based hybrid sorbents, and (5) important factors (pore size and surface chemistry) influencing CO2 uptake over carbon adsorbents. Further, the future prospects of carbon-based adsorbents are briefly discussed.