K9 optical glass has an important position in the field of optical material because of its excellent chemical stability and optical projection. The hard and brittle characteristics of K9 optical glass make conventional processing difficult and time-consuming. A non-conventional hybrid polishing system combining ultrasonic atomization (UA) spraying method and axial ultrasonic vibration was developed for processing K9 optical glass. This system utilizes the high-frequency vibration characteristics of ultrasonic vibration technology: On the one hand, the ultrasonic atomization spraying method is used to generate evenly distributed atomized droplets for polishing, on the other hand, the axial ultrasonic vibration of the polishing tool provides impact kinetic energy for the free abrasive particles. Mechanical polishing (MP), ultrasonic-assisted polishing (UVP), mechanical polishing under ultrasonic atomization spraying (UA-MP) and ultrasonic vibration polishing under ultrasonic atomization spraying (UA-UVP) were carried out on K9 optical glass. The material removal rate (MRR), material removal depth (MRD), surface quality and surface micromorphology of the polished workpieces were also analyzed and compared. The experimental results showed that the best surface was obtained at UA-UVP (AⅠ = 9 μm) with MRR of 0.0994 mm3/min, material removal depth of 26.816 μm, the Ra and Sa values were 0.028 μm and 0.033 μm respectively. Meanwhile, no obvious pits and scratches were observed on the micromorphological surface. Ultrasonic atomization contributes to even material removal from the polished surface and axial ultrasonic vibration of the polishing tool has a significant effect in improving the polishing characteristics, which provides the experimental basis for applying ultrasonic vibration technology in polishing.