Clean energy sources and global warming are among the major challenges of the 21st century. One of the possible actions toward finding alternative energy sources and reducing global warming are storage of H2 and CH4, and capture of CO2 by using highly efficient and low-cost adsorbents. Graphene and graphene-based materials attracted a great attention around the world because of their potential for a variety applications ranging from electronics, gas sensing, energy storage and CO2 capture. Large specific surface area of these materials up to ~3000m2/g and versatile modification make them excellent adsorbents for diverse applications. Here, graphene-based adsorbents are reviewed with special emphasis on their adsorption affinity toward CO2, H2 and CH4. This review shows that graphene derivatives obtained mainly via “chemical exfoliation” of graphite and further modification with polymers and/or metal species can be very effective sorbents for CO2 and other gases and can compete with the currently used carbonaceous or non-carbonaceous adsorbents. The high adsorption capacities of graphene-based materials are mainly determined by their unique nanostructures, high specific surface areas and tailorable surface properties, which make them suitable for storage or capture of various molecules relevant for environmental and energy-related applications. Display omitted •Tuning adsorption properties of graphene by coupling with nanoparticles•Appraisal of properties of graphene materials for CO2, H2 and CH4 adsorption•Comparison of gas adsorption affinity for graphene, activated carbons and MOFs