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A series of four isostructural microporous coordination polymers (MCPs) differing in metal composition is demonstrated to exhibit exceptional uptake of CO₂ at low pressures and ambient temperature. These conditions are particularly relevant for capture of flue gas from coal-fired power plants. A magnesium-based material is presented that is the highest surface area magnesium MCP yet reported and displays ultrahigh affinity based on heat of adsorption for CO₂. This study demonstrates that physisorptive materials can achieve affinities and capacities competitive with amine sorbents while greatly reducing the energy cost associated with regeneration.