This study investigated CO2 absorption into K2CO3 solution enhanced by cyclohexane in a novel high-gravity device named a high-shear reactor (HSR). CO2 absorption percentage and enhancement factor in both the cyclohexane/K2CO3 emulsion and the K2CO3 solution were measured to assess the influence of cyclohexane. The effect of various operating parameters including the volume fraction of cyclohexane, rotation speed of HSR, gas and liquid volumetric flow rates, and liquid temperature was investigated. It was observed that HSR can intensify the absorption of CO2 markedly. The effective interfacial area of the gas-liquid-liquid system in the HSR was calculated to reveal the enhancement mechanism of the organic phase. The results indicate that addition of cyclohexane increased the interfacial area of the gas-liquid-liquid system in the HSR, which was favorable for the gas-liquid mass transfer process and thus significantly enhanced CO2 absorption efficiency.