Experiments on carbon black production from coal tar via chemical looping pyrolysis were performed in a fluidized bed reactor using natural hematite, hematite/gamma-Al2O3 (Fe/Al), and hematite/NiO (Fe/Ni) composites as oxygen carriers (OCs). After 3 redox cycles, thermogravimetric analysis combined with differential scanning calorimetry results show that, in comparison to natural hematite, the oxidation rate of the Fe/Al OC became faster above 700 degrees C; however, the oxidation performance of the Fe/Ni OC was always poor. The addition of gamma-Al2O3 could effectively inhibit carbon deposition; nonetheless, NiO exhibited the opposite effect. On the basis of the burning temperature, the carbon deposition on reduced OCs was mainly hard coke. The X-ray diffraction analysis showed that NiO was not only more effective than gamma-Al2O3 to promote the reduction of Fe2O3 in compound OCs but also increased the sintering trend. The scanning electron microscopy analysis indicated the melting of original grains at the surface of the hematite OC under a high temperature, and the surface sintering was serious. However, the Fe/Al OC always exhibited a relatively stable porous structure; thus, the sintering was alleviated as a result of gamma-Al2O3 addition. Owing to the weak mechanical strength, the Fe/Ni OC cracked after 3 cycles, leading to deposition of a large amount of coke, and its surface sintering was more serious compared to that of the hematite OC.