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Industrial hydrocarbon separations are performed on an immense scale, accounting for a significant fraction of global energy consumption. Supplanting thermally driven separation processes (e.g., distillation) with adsorbent-based technologies could greatly reduce energy expenditures and production costs associated with these commodity chemicals. Significant effort has been expended towards the development of metal–organic frameworks (MOFs) as adsorbents for this purpose, owing to their high surface areas and crystallinity, as well as their structural and chemical tunability. This review presents some of the recent progress made in MOF material design to accomplish separations of C_2–3 hydrocarbons, which are crucial to the production of high-grade ethylene and propylene.