Graphene-based materials have generated tremendous interest in a wide range of research activities. A wide variety of graphene related materials have been synthesised for potential applications in electronics, energy storage, catalysis, and gas sorption, storage, separation and sensing. Recently, gas sorption, storage and separation in porous nanocarbons and metal-organic frameworks have received increasing attention. In particular, the tuneable porosity, surface area and functionality of the lightweight and stable graphene-based materials open up great scope for those applications. Such structural features can be achieved by the design and control of the synthesis routes. Here, we highlight recent progresses and challenges in the syntheses of graphene-based materials with hierarchical pore structures, tuneable high surface area, chemical doping and surface functionalization for gas (H2, CH4, CO2, N2, NH3, NO2, H2S, SO2, etc.) sorption, storage and separation.