Simultaneous absorption of the acid gas CO2 and a volatile organic compound (VOC; here n-hexane) from a polluted gas stream by using an emulsion in a gas-liquid-liquid (GLL) reactor was investigated. In order to enhance the VOC capture, a nonaqueous liquid phase in the form of silicone oil was applied in the gas absorber. In addition, the regeneration process of both liquid phases was analyzed. The effect of methyldiethanolamine concentration in the aqueous phase and percentage of the organic phase was evaluated, showing opposite results for the liquid phases regarding each gas due to the differences between them. A higher amount of silicone oil causes a significant improvement in VOC absorption rate with negligible influence on CO2 behavior. The gas composition was modified by nitrogen.