Abstract: The accelerating rise in global carbon dioxide emissions underscores the urgency of developing efficient direct air capture (DAC) technologies. Metal-organic frameworks (MOFs), owing to their structural tunability, high surface area, and excellent stability, exhibit great potential for low-concentration CO2 capture. This review systematically summarizes recent progress in the structural design and modification strategies of MOFs for DAC applications from four perspectives. The importance of amine functionalization in enhancing CO2 capture performance is elucidated, including both grafting and impregnation approaches, as well as the improved performance observed under humid conditions. Meanwhile, the limitations of these strategies in terms of stability are also discussed. Furthermore, regulation strategies involving metal nodes and organic linkers are summarized, such as the introduction of open metal sites, metal-ligand synergistic effects, polar ligand and heteroatom modifications, and defect engineering. Strategies to enhance the hydrophobic stability of MOFs, including fluorination and hydrophobic modifications, core-shell structure construction, and interfacial hydrophobic regulation, are also introduced. Finally, the review discusses composite approaches combining MOFs with polymers and other materials, aiming to overcome the engineering limitations of powder-form materials and promote their practical application. Despite the remaining challenges of stability, shaping, and large-scale synthesis in practical DAC applications, MOFs, with their exceptional structural tunability and functional diversity, remain among the most promising materials for carbon capture. Through synergistic design at both the molecular and structural levels, a balance between adsorption capacity, stability, and energy efficiency can be achieved. With the continuous advancement of material design concepts and processing technologies, MOFs are expected to play a significant role in DAC systems, providing strong support for achieving carbon neutrality.