Composite materials for carbon dioxide (C02) capture that include: (1) a mesoporous carbon source; and (2) an in situ polymerized polymer that is associated with the mesoporous carbon source, where the in situ polymerized polymer is selected from the group consisting of thiol-based polymers, amine-based polymers, and combinations thereof. Methods of making the composite materials for C02 capture include: (1) associating a mesoporous carbon source with monomers, where the monomers are selected from the group consisting of thiol-based monomers, amine-based monomers, and combinations thereof; and (2) polymerizing the monomers in situ to form said composite materials. Further embodiments of the present invention pertain to methods of capturing C02 from an environment by associating the environment with one or more of the aforementioned composite materials.