A piece of diamond film (Ø 125 mm) was polished based on prefabricated stress. The diamond film was glued to a metal workpiece at high temperatures. The difference in the thermal expansion coefficients between the diamond film and the workpiece was exploited to prefabricate stress in the middle of the two materials. This prefabricated stress had a compressive effect on the diamond film, offset the stress generated in the grinding and polishing process, and prevented the diamond film from cracking. The feasibility of the prestressing method was verified by a combination of experiments and finite element simulations. The prestressing method was used to bond the diamond film to a 10 mm-thick brass fixture at 20, 50, 70, and 90 °C. It was found that when the temperature of the bonded diamond film reached 90 °C, the increase in the prefabricated stress was −410.71 MPa. The finite element simulation results were found to be consistent with the experimental data. The diamond film was cooled down to room temperature after bonding at high temperatures to simulate the prefabricated stress generation process. The diamond film with the prefabricated stress was again heated to the bonding temperature to simulate the stress change caused by the frictional heat generated during the polishing process. The stress of the bonded sample increased when it was cooled down to room temperature. The stress on the diamond surface became smaller during the polishing process, and the stress almost disappeared with the rise in bonding temperature, verifying the viability of the prestressing method.