Grapefruit seeds were studied for the extraction of limonoids using supercritical CO2 extraction (SC-CO2) technique. Limonin aglycone was successfully extracted with SC-CO2 directly from grapefruit seeds; and the limonin glycoside was extracted using SC-CO2 and ethanol as co-solvent from the spent seeds after the extraction of limonin aglycone. In an effort to optimize the extraction conditions of limonin aglycone, pressure, temperature, time effects were investigated. Various times of extraction, CO2 flow rate and the feeding modes of CO2 were also employed to obtain the highest yield of limonin aglycone. Optimal conditions to achieve the highest limonin aglycone (0.63 mg/g seeds) were 48.3 MPa, 50°C and 60 min with CO2 bottom feeding, flow rate about 5 L/min. The extraction conditions for limonin glycoside to achieve highest yield were further optimized. The highest extraction yield (0.62 mg limonin glycoside/g seeds) were at 48.3 MPa, 50°C, 30% molar fraction of ethanol (XEth =0.30) and 40 min with CO2 top feeding, flow rate about 5 L/min. The results demonstrated that supercritical CO2 extraction of limonoids from grapefruit seeds, a citrus juice industry byproduct, has practical significance for commercial production.