Sapphire ultrasonic vibration-assisted flexible polishing (UVAFP) is a promising technique for comprehensively improving the surface integrity of machined parts. The technique was performed on an ultra-precision machine tool with the in-situ monitoring systems in this paper, which aims to provide a new perspective for understanding the material removal mechanisms in the sapphire UVAFP process. A Taguchi L 9 (4 3 ) orthogonal experiment was conducted to investigate the effects of feed distance, spindle speed, ultrasonic vibration (UV), and polishing time on the surface finish and material removal in the process. In addition, the effect of a polyurethane ball tool is not trivial. A single-factor experiment was conducted for exploring it. Based on a laser displacement measurement system and an acoustic emission sensor system, the characteristics of time-dependent ultrasonic amplitude and ultrasonic frequency for the sapphire UVAFP system were analyzed, with the effectiveness of UV demonstrated. Based on a three-component force measurement system, the characteristics of normal force and its relationship with process parameters and tool deformation were analyzed, with macro- and micro-level examined. In conclusion, this paper presents the characterization of UV and polishing force in the sapphire UVAFP process, providing novel insights into understanding the material removal mechanisms of sapphire and even more manufacturing problems.