The facile uptake of CO2 gas in a nonporous molecular crystal constituted by long molecules with carbazole and ethynylphenyl moieties was reported in experiments recently. Herein, the mechanism of gas uptake by this crystal is elucidated using atomistic molecular simulations. The uptake of CO2 is shown to be facilitated by (i) the capacity of the crystal to expand in volume because of weak intermolecular interactions, (ii) the parallel orientation of the long molecules in the crystal, and (iii) the ability of the molecule to marginally bend, yet not lose crystallinity because of the anchoring of the terminal carbazole groups. The retention of crystallinity upon sorption and desorption cycles is also demonstrated. At high enough pressures, near-neighbor CO2 molecules sorbed in the crystal are found to be oriented parallel to each other.