A novel calcium looping (CaL) process integrated with a spent bleaching clay (SBC) treatment is proposed whereby fuels and/or heat from regeneration of SBC provide supplemental energy for the calcination process; in addition, the regenerated SBC could be used to synthesize enhanced CaO-based sorbents. Composite samples were prepared with various doping ratios together with the regenerated SBC via a pelletization process. All pellets were subjected to thermogravimetic analysis (TGA) tests employing severe reaction conditions to determine the optimal doping ratios and regeneration method for the SBC-based sorbents. These results demonstrate that pellets containing combustible components showed higher CO 2 uptake, due to the improved pore structure, which was verified by N 2 adsorption measurements. The as-prepared sorbent "L-10PC" (90% CaO/10% pyrolytic SBC) achieved a final CO 2 uptake of 0.164 g(CO 2) g(calcined sorbent)-1 after 20 cycles, which was 67.3% higher than that of natural limestone particles. A new larnite (Ca 2 SiO 4) phase was detected by XRD analysis; however, the weak XRD peak associated with it indicated a low content of larnite in the pellets, which produced a smaller effect on performance compared to cement. A synergistic effect was achieved for a sample designated as "L-5PC-10CA" (85% CaO/5% pyrolytic SBC/10% cement), which resulted in the highest final uptake of 0.208 g(CO 2) g(calcined sorbent)-1. Considering the simplicity of the pyrolysis regeneration process and the excellent capture capability of pellets doped with pyrolytic SBC, the proposed system integrating CaL with SBC pyrolysis treatment appears to be promising for further development.