<p>Although there is an urgent demand for high-quality polished surfaces, conventional manufacturing techniques are frequently constrained by high production costs and low processing efficiency. Therefore, this study proposes a new harmonic vibration-assisted magnetorheological polishing (HVMRP) method to investigate the influence of two-dimensional harmonic vibration on the abrasive trajectory, microscale material removal, and its impact on the machining performance of K9 optical glass. The abrasive trajectory of the magnetorheological influenced region is investigated, demonstrating that non-integer speed ratios can effectively enhance the distribution uniformity and coverage density of the abrasive trajectory. Meanwhile, a normal force model (comprising magnetic normal force, fluid dynamic pressure, and normal impact force) and a material removal model are constructed sequentially. The normal impact force coefficient is quantitatively determined through experimental curve fitting. Furthermore, an HVMRP surface topography with abrasive trajectory is predicted, and the rationality and practicality of the proposed HVMRP surface generation mechanism are verified through experiments. The relative error of the model prediction accuracy remains within 15%. The results show that the harmonic vibration can effectively enhance both the material removal efficiency and the surface quality. This study provides a new approach for efficient and precise machining of optical glass and other brittle-hard materials.</p>