The anticipated significant use of lithium-ion batteries (LIBs) for energy storage applications in electric grid modernization and vehicle electrification shall generate a large quantity of solid waste that could become potential environmental hazards and waste natural resources. Recycling of the major components from spent LIBs is, therefore, considered desirable to prevent environmental pollution and to recycle valuable metals. This study reports on the application of ultrasonic-assisted technology to the leaching of cobalt and lithium from the cathode active materials of spent LIBs. Three acids were tested for the leaching process: two inorganic acids (H2SO4 and HCl) and one organic acid (citric acid, C6H8O7·H2O). The results show that the leaching of Co and Li is more efficient with citric acid than with the two inorganic acids. More than 96% Co and nearly 100% Li were recovered from spent LIBs. The optimal leaching conditions were 0.5 M citric acid with 0.55 M H2O2, a solid-to-liquid ratio of 25 g L−1, a temperature of 60 °C, leaching time of 5 h, and ultrasonic power of 90 W. The high leaching efficiency is mainly ascribed to the unique cavitation action of the ultrasonic waves. This ultrasonic-assisted leaching process with organic acid is not only effective but also environmentally friendly.