Novel nanoparticle organic hybrid materials (NOHMs), which are comprised of organic oligomers or polymers tethered to an inorganic nanosized cores of various sizes, have been synthesized, and their solvating property for CO2 was investigated using attenuated total reflectance (ATR) Fourier transform infrared (FT-IR) spectroscopy. Simultaneous measurements of CO2 capture capacity and swelling behaviors of polyetheramine (Jeffamine M-2070) and its corresponding NOHMs (NOHM-I-PE2070) were reported at temperatures of (298, 308, 323 and 353) K and CO2 pressure conditions ranging from (0 to 5.5) MPa. The polymeric canopy, or polymer bound to the nanoparticle surface, showed significantly less swelling behavior with enhanced or comparable CO2 capture capacity compared to pure unbound polyetheramine.