Aiming at problems such as poor precision of laser processing C/SiC composites, low efficiency of grinding C/SiC composites, and serious wear of grinding wheel, a method of laser-grinding chain processing C/SiC composite groove was proposed in this paper. The method combined the high efficiency characteristic of laser ablating and the high precision characteristic of grinding. The relationship between laser processing parameters and the characteristics of ablative grooves was investigated, and the appropriate laser processing parameters were optimized, and then, to further improve the processing quality of the grooves, the grinding parameters optimization experiments of the grooves of C/SiC composites were carried out. The results showed that the C/SiC composites could be quickly removed by laser processing, and the grooves with relatively good size and shape accuracy could be obtained by laser parameters optimization experiments, but the side wall of the groove still had a certain inclination and the surface quality of the groove was yet poor; meanwhile, the size accuracy, shape accuracy, and surface quality of the grooves were greatly improved by further grinding. In addition, then, through the laser and grinding optimization experiments, the optimized parameters were obtained, where the laser power was 80 W, the scanning speed was 300 mm/s, the scanning frequency was 50 kHz, the scanning spacing was 25 μm, the depth of cut was 30 μm, the liner speed of wheel was 62.832 m/min, and the feed speed was 10 mm/min. With these parameters, the time used to process the groove with the laser-grinding chain was about 23/40 of the grinding process, and the quality of grooves could be guaranteed. Therefore, combined with the optimized process parameters, the laser-grinding chain processing scheme could be used to achieve high efficiency and precision grinding of C/SiC composite grooves.