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CO₂ represents a typical impurity in light hydrocarbon feedstocks, which affects the quality of subsequent chemical products. Owing to their highly similar nature, industrial separation requires large amounts of energy. Adsorptive gas separation based on porous materials is considered an efficient alternative, as it can offer faster kinetics, higher selectivity, long-term stability and more energy-efficient regeneration. For the adsorption separation method, preferential CO₂ capture from gas mixtures in one step is more energy-efficient for direct purification than light hydrocarbons, saving about 40% energy by eliminating energy-intensive post-regeneration processes such as countercurrent vacuum blowdown. Therefore, CO₂-selective adsorbents are more sought-after than light hydrocarbon-selective adsorbents. Metal-organic frameworks (MOFs) have been demonstrated as outstanding physisorbents for CO₂ capture due to their configurable channels for CO₂ recognition, structural flexibility and large specific surface area. Many highly selective CO₂ adsorption behaviors of MOFs have been reportedly achieved by precise modulation of pore size, pore chemistry or structural flexibility. In this review, we discuss the emerging development of MOFs for CO₂-selective capture from different light hydrocarbon mixtures. The challenges of CO₂ recognition and the strategies employed to achieve CO₂ selectivity over light hydrocarbon mixtures by MOFs are summarized. In addition, the current challenges and prospects in the field of MOFs for CO₂ capture are discussed and elaborated.