This chapter discusses the importance of carbon capture and the need for developing materials that can cover the disadvantages held by current conventional substances for carbon capture. Furthermore, evaluations are made for more environmentally friendly responses and to lower the end costs of a process by using carbon-based materials. Carbon capture and sequestration include several phases, which begin with capturing the carbon and then separating it from the system before further operations. Carbon-based materials can successfully be implemented in different stages of CO2 sequestration, which is due to their tunable nature. Nevertheless, this chapter primarily focuses on separation stage since it allows for novelty in terms of applied materials. Specifically, two of the most used processes for CO2 separation including adsorption and membrane systems could be well enhanced by implementing such materials. Materials such as activated carbon, biochar, graphene, and carbon nanotubes have gained attention over the last two decades, and their large-scale application is growing gradually. Technical evaluations of using such materials in these systems are considered from different aspects as a pre-requirement in a large-scale application. Finally, despite carbon capture strategies using carbon-based materials are theoretically proving to be efficient in different aspects, their actual benefits when seen in a larger framework should be assessed carefully. Carbon capture by nature can be a big step toward climate change actions that are set for the upcoming years; however, as for a short time solution, they cannot guarantee a robust response. In addition, the environmental costs for setting up the carbon capture equipment need to be studied in comparison to the existing power plants before decision-making.