A series of porous core-membrane microstructured nanomaterials, constructed of a deep eutectic solvent (DES) membrane and porous MOF-808 core via liquid surface tensions and electrostatic interactions, are introduced for carbon dioxide capture with the sorption mechanism coupling diffusion, physisorption, and chemisorption. MOF-808 as the porous core considerably improves the diffusion interactions for DES membranes, hence significantly enhancing the sorption performance of DESs. Although the DES consisted by monoethanolamine and tetrapropylammonium chloride (MEA-TPAC-7) has the highest sorption capacity among all DESs, it is only 4.39 mmol g-1 at 2.4 bar and further attenuates by fastidious diffusion interactions when increasing viscosity or dose. The sorption capacities of DES@MOF-120 are 5.18 mmol g-1 at 3.0 bar and 4.78 mmol g-1 at 2.4 bar without apparent sorption hysteresis in pressure swing sorption, which are substantially improved contrasted to MEA-TPAC-7. The sorption isotherms are reconstructed via Sips models considering surface heterogeneity with regression correlation coefficients over 0.9454 to forecast maximum sorption capacity over 6.33 mmol g-1 .