In this study, the gas phase volumetric overall mass transfer coefficients (K G a e ) for CO 2 absorption into aqueous ammonia solutions were measured to explore the mass transfer performance of a column packed with structured packing. The K G a e values were evaluated over ranges of main operating variables, that are, 1400−2300 m 3 ·m −2 ·h −1 gas flow rate, 20−39 m 3 · m −2 ·h −1 liquid flow rate, up to 8 kPa partial pressure of CO 2 , and 0.27−0.72 kmol·m −3 ammonia concentration. The results show that higher liquid loading and concentration of aqueous ammonia are beneficial to enhance the K G a e values. On the contrary, K G a e value decreases as the CO 2 partial pressure increases. The results also show that gas loading has little influence on K G a e . To allow the mass transfer data to be readily utilized, an empirical K G a e correlation for this system was developed. Finally, Simulations were made for the absorption of CO 2 into aqueous ammonia solutions by using the currently developed computational mass transfer model along with the proposed correlation for K G a e . The simulation results on the gas phase CO 2 concentration are found to be in satisfactory agreement with the experimental measurements.