In the grinding process, acceleration signals in both the time and frequency domains are valuable for monitoring and controlling vibration patterns, as factors such as rotational speed and the grinding head design significantly influence machining quality, efficiency, and finishing performance. This study analyzes the acceleration signals by dividing them into three distinct stages, pairing this analysis with microscopic morphology to investigate the grinding behavior of carbon fiber-reinforced polymer (CFRP). The findings reveal that high-frequency and low-amplitude vibrations enhance polishing efficiency and quality, whereas low-frequency and high amplitudes adversely affect grinding quality. Acceleration vibrations are more stable during the intermediate grinding stage compared to the initial and final stages, which helps reduce surface roughness, regardless of the rotational speed or grinding head mesh size. In addition, a coarse mesh (#40) results in an uneven surface due to a large amount of removed material, whereas a fine one (#120) results in lower material removal but continuous vertical vibrations due to the impact with the grinding surface, also resulting in poor surface quality. Thus, controlling the tool’s size and rotational speed is essential in reducing the amplitude of the vibration, allowing for maximizing the grinded CFRP surface quality.