Metal–organic frameworks (MOFs) offer unprecedented atom-scale design and structural tunability, largely due to the vast number of possible organic linkers which can be utilized in their assembly. Exploration of this space of linkers allows identification of ranges of achievable material properties as well as discovery of optimal materials for a given application. Experimental exploration of the linker space has to date been quite limited due to the cost and complexity of synthesis, while high-throughput computational studies have mainly explored MOF materials based on known or readily available linkers. Here an evolutionary algorithm for de novo design of organic linkers for metal–organic frameworks is used to predict MOFs with either high methane deliverable capacity or methane accessible surface area. Known chemical reactions are applied in silico to a population of linkers to discover these MOFs. Through this design strategy, MOF candidates are found in the ten symmetric networks acs, cds, dia, hxg, lvt, nbo, pcu, rhr, sod, and tbo. The correlation between deliverable capacities and surface area is network dependent.