The storage and selective binding of fuel and contaminant gases in a safe and compact form represents a significant current challenge. There is wide-ranging interest in the development of stable porous materials that can store, release and purify H2, CO2, SO2, NO2, CH4 and hydrocarbons with fast kinetics and high reversibility over multiple cycles. The synthesis, structural characterisation and gas adsorption studies of a range of porous metal-organic materials showing high storage capacities and selectivities will be discussed. Of particular interest arein situ structural and dynamic studies of gas-loaded materials that define the binding of substrates within pores at a molecular level. Powder and single crystal X-ray and neutron diffraction and inelastic neutron scattering (INS) studies, combined with density functional theory (DFT) modelling, reveal a range of host-guest supramolecular hydrogen bonding and ?-? contacts that enable the selective binding of substrates. This offers exciting potential for the application of new capture systems based on the soft binding via the use of an “easy-on” and “easy-off” model.