Highly mesoporous LTA zeolite (Meso-LTA) was prepared using an organosilane surfactant, dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride, as a mesopore-generating agent. Meso-LTA was characterized by X-ray powder diffraction, N-2 adsorption-desorption isotherm at 77 K, scanning electron microscopy equipped with an energy dispersive X-ray spectroscopy, and then investigated for CO2 adsorption at 298 K. Compared to a solely microporous LTA zeolite (Micro-LTA), Meso-LTA showed faster CO2 adsorption kinetics at 1 bar and higher CO2 adsorption capacities under high pressure conditions (>10 bar). 2014 Elsevier B.V. All rights reserved.