To realize high-efficiency CO2 absorption by fresh cement paste, ultrasonic vibration technology is introduced into the CO2 absorption test device used in this study. Influences of ultrasonic frequency on the CO2 absorption rate (CO2 AR) and the ultimate absorption amount of fresh cement paste are analyzed. Furthermore, the influencing laws of the CO2 absorption amount (CO2 AA) on the fluidity, pore distribution, and mechanical properties of cement paste under ultrasonic vibrating agitation are analyzed by measuring the variations of the CO2 AA of cement paste. Results demonstrate that ultrasonic vibrating agitation not only can increase the CO2 AR and ultimate absorption amount of fresh cement paste, but also can optimize the internal pore structure of materials and compressive strength of cement-based materials.