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Metal–organic frameworks (MOFs) have diverse applications involving the storage, separation and sensing of weakly interacting, high-purity gases. Exposure to impure gas streams and interactions with corrosive and coordinating gases raises the question of chemical robustness; however, the factors that determine the stability of MOFs are not fully understood. Framework materials have been previously categorized as either thermodynamically or kinetically stable, but recent work has elucidated an energetic penalty for porosity for all these materials with respect to a dense phase, which has implications for the design of materials for gas storage, heterogeneous catalysis and electronic applications. In this Review, we focus on two main strategies for stabilization of the porous phase — using inert metal ions or increasing the heterolytic metal–ligand bond strength. We review the progress in designing robust materials …