The globally increasing concentrations of greenhouse gases in atmosphere after combustion of coal-or petroleum-based fuels give rise to tremendous interest in searching for porous materials to efficiently capture carbon dioxide (CO2) and store methane (CH4), where the latter is a kind of clean energy source with abundant reserves and lower CO2 emission. Hundreds of thousands of porous materials can be enrolled on the candidate list, but how to quickly identify the really promising ones, or even evolve materials (namely, rational design high-performing can-didates) based on the large database of present porous materials? In this context, high-throughput computational techniques, which have emerged in the past few years as powerful tools, make the targets of fast evaluation of adsorbents and evolving materials for CO2 capture and CH4 storage feasible. This review provides an overview of the recent computational efforts on such related topics and discusses the further development in this field.