Elastic spherical polishing tools effectively conform to the polishing surface and exhibit high efficiency in the removal of materials, so they are extensively used in the sub-aperture polishing stages of optical components. However, their processing is often accompanied by significant mid-spatial frequency (MSF) errors, which critically degrade the performance of optical systems. To suppress the MSF errors generated during polishing with spherical tools, this study investigates the influence factor of MSF errors during the polishing process through an analysis of the convolution effect in material removal. A material removal profile model is established, and a uniform removal simulation is conducted to assess the influence of different shape material removal profiles on MSF errors. Simulation and experimental results show that a Gaussian-like shape material removal profile is more effective in suppressing the MSF errors during polishing compared to the “W” and trapezoidal shape material removal profiles. In addition, based on the characteristics of the RMS decreasing in a serrated trend with the decrease in path spacing, a path spacing optimization method considering the polishing efficiency is proposed to improve the polishing efficiency while controlling the MSF errors, and the effectiveness of the path spacing optimization method is verified by comparing the MSF error at the maximum theoretical path spacing and the path spacing that is less than this. Finally, the path spacing optimization method is used to polish single-crystal silicon to further illustrate its practicality.