Clean and renewable energy and technologies are in great demand due to environmental and energy concerns. Hydrogen (H 2 ) and natural gas (NG, mainly methane) are more environmentally friendly and efficient alternative fuels given their lower exhaust emissions and high gravimetric energy densities. Compared with conventional fossil fuels, the combustion of hydrogen emits only water, while natural gas emits 25% less carbon dioxide. For hydrogen and methane, their gravimetric heats of combustion (123 and 55.7 MJ kg À1 , respectively) are higher than that of gasoline (47.2 MJ kg À1 ) (Suh et al., 2012). These advantages make hydrogen and methane promising clean power sources. However, the density of either hydrogen or methane is extremely low, making their onboard storage a great challenge and preventing the widespread use of these gases in vehicles. Possible solutions in conventional storage could be liquefaction at low temperature (20 K for liquefied hydrogen) or compression at ambient temperature and high pressure (hundreds of atmospheres). These solutions require heavy bulky fuel tanks or expensive compressors, putting a serious limitation on their possible applications, particularly for passenger vehicles. An alternative solution is to increase the gas storage density under relatively mild conditions using porous materials. Introducing porous materials into fuel tanks can drastically reduce the stored pressure at ambient temperature, which is more efficient and safe. Hence it is critically important to develop efficient adsorbent materials to use these promising clean fuels.Metal-organic frameworks (MOFs, also known as porous coordination polymers) are a new generation of porous materials (Furukawa et al., 2013) which have intensively changed a wide range of technological fields, especially in the separation and storage of gases. Owing to their uniform pore structures, tunable pore sizes and designable structures, MOFs have been proven as ideal candidates for hydrogen and methane storage (Suh et al., 2012;Li et al., 2016;He et al., 2014;Mason et al., 2014;Sculley et al., 2011). Benefitting from the infinite permutations of their inorganic and organic components, MOFs are more extensive in their diversity than any other class of conventional porous material. The pore structures are easily controlled to obtain optimized performance, which has been clearly demonstrated in the latest important progress on MOFs for hydrocarbon separation (Cui et al., 2016). MOFs were first reported to store hydrogen gas in around 2003(Rosi et al., 2003, while methane storage can be dated back to 1997 (Kondo et al., 1997). Since then, remarkable progress has been achieved and hundreds of MOFs have been developed with a high capacity for these fuel gases.Generally, the interaction between hydrogen and the surface of a MOF is quite weak, so functionalizing the organic linkers will have little positive effect on hydrogen adsorption. By increasing the pore volume and surface area, the total gravimetric hydrogen capacity can be up to 17....