New materials capable of separating mixtures of saturated, unsaturated, and aromatic hydrocarbons can enable more efficient industrial processes and cleaner energy. Outstanding challenges in hydrocarbon separations stem from the similar structures, properties, and reactivities of the molecules comprising many of these mixtures. With high surface areas, tunable pore geometries, and adjustable surface functionality, metal–organic frameworks hold tremendous promise for effecting previously difficult or impossible separations. In this review, we provide a comprehensive account of the metal–organic frameworks that have been investigated for hydrocarbon separations within the context of their potential relevance for separating various industrial alkane-, alkene-, and aromatic-containing mixtures.