Our group published a review on metal-organic framework-based CO2 capture. CO2 capture is a hot topic in research and industry. It typically refers to the splitting of CO2/N2, H2/CO2 and CO2/CH4, and is one of the most desirable separation technologies in environment and energy sectors. Membrane-based separations are energy-efficient separation methods cutting the energy consumption of traditional distillation by nearly 90%, which offers hope for CO2 capture. Metal-organic frameworks (MOFs) are a versatile platform with compositional and structural tunability, lighting the concept from precise material design to membranes for high-efficiency CO2 capture. This review provides readers with a comprehensive overview. We summarized compositional/structural design and regulation strategies of MOFs targeted at secondary building units (metal nodes and linkers), pore structure, topology and mixed-phase hybrid structures for achieving CO2-philic MOF materials. And diversified methods were illustrated for construction of improved MOF membranes that can overcome the bottleneck of permeability-selectivity limitations.This work has been published in Frontiers of Chemical Science and Engineering as a cover paper, 2020, 14, 188-215