A gas cyclone–liquid jet absorption separator integrates the functions of cyclone separation, liquid jet atomization, and absorption separation. This study employed this device to conduct a wet flue-gas desulfurization experiment on a gas mixture consisting of air in room temperature and sulfur dioxide (SO2) to explore this device’s prospect of tail gas purification. Sodium hydroxide (NaOH) and sodium carbonate (Na2CO3) solutions at various concentrations were used as absorbents under room temperature. The changes in the SO2 removal efficiency and air pressure drop were investigated with parameters including total gas flow, SO2 concentration in the flue gas, and absorbent flow. The SO2 removal efficiency increased to a certain extent as the absorbent concentration, total gas flow, and absorbent flow increased. The maximum SO2 removal efficiencies of NaOH and Na2CO3 were 85% and 77%, respectively. Under identical experimental conditions, the changes in SO2 removal efficiencies of NaOH and Na2CO3 exhibited essentially identical trends, in which NaOH exhibited a 5%–8% greater SO2 removal efficiency than Na2CO3.