Grand-canonical Monte Carlo simulations and adsorption experiments are combined to fnd the optimized carbon nanotube (CNT) arrays for gas adsorption at low pressures and 303 K. Bundles of 3D aligned double-walled carbon nanotube (DWCNT) with inner diameter of 8 nm and di?erent intertube distances were made experimentally. The experimental results show that decreasing intertube distance leads to a signifcant enhancement in carbon-dioxide (CO2) adsorption capacity at 1 bar. The molecular simulation study on CO2 adsorption onto bundles of 3D aligned DWCNT with inner diameters of 1, 3, and 8 nm and intertube distance of 0-15 nm shows that the intertube distance plays a more important role than the CNT diameter. The simulation results show that decreasing the intertube distance up to 1 nm increases the excess adsorption generally in all the studied systems at pressures 0 < p < 14 bars (the increase can be up to ∼40% depending on the system and pressure). This is in agreement with the experimental result. Further reduction in intertube distance leads to a decrease in the excess adsorption in the pressure range 9 < p < 14 bars. However, at lower pressure, 0 < p < 9 bars, intertube distance of 0.5 nm is found to have the highest excess adsorption. This result is indifferent to tube diameter. Furthermore, molecular simulations are conducted to obtain the optimal parameters, for the DWCNT bundle, for SO2 adsorption, which are similar to those observed for CO2 in the pressure range 0 < p < 3 bars. © 2015 AIP Publishing LLC.