Abstract: Light-responsive adsorbents have been extensively studied as a new class of smart adsorption materials. The photo-responsive adsorption process can be precisely controlled by external light, offering the advantages of remote controllability and low energy consumption in CO2 capture. The light-controlled regulation of photo-responsive adsorbents stems from the functionalization of their photo-responsive units. Metal-organic frameworks (MOFs) are highly suitable for the functionalization of light-responsive units due to their high specific surface area, tunable pore sizes, and ease of surface modification. Common light-responsive MOF adsorbents incorporate light-responsive units such as azobenzene, diarylethylene and spiropyran into their frameworks. Under excitation by light of specific wavelengths, these units undergo reversible photoisomerization reactions, which precisely regulate the pore size, shape, and distribution of surface adsorption sites within the MOFs, ultimately enabling flexible control over CO2 adsorption capacity and selectivity. The adsorption process in light-responsive MOFs is regulated through the synergistic action of multiple mechanisms, primarily including: spatial steric effects resulting from photodriven conformational changes of ligands, which alter the pore microenvironment; differences in polarity before and after ligand isomerization, which influence the strength of interactions with CO2; dynamic adjustments in the number and adsorption strength of adsorption sites through interactions with light-responsive units; light-induced electron transfer, which alters the material’s electronic structure and enhances adsorption affinity; and the light-induced thermal effect, which indirectly regulates the system temperature to assist in controlling the adsorption-desorption process. Although light-responsive MOF adsorbents offer significant advantages in CO2 capture, they currently face bottlenecks such as limited light penetration depth, confinement to ultraviolet wavelengths, and insufficient long-term cycling stability. Current research primarily focuses on optimizing visible/infrared light responsiveness, synergistic binding with auxiliary ligands, and composite grafting with traditional adsorbent matrices. In the future, with continuous improvements in the design and preparation of light-responsive materials, light-responsive MOFs are expected to overcome existing bottlenecks, achieve broader applications in carbon capture, and provide crucial material support and technological assurance for the realization of global carbon neutrality goals.