The utilization of sulfur acid residue is an urgent problem confronting sulfuric acid production enterprises, especially the application of sulfur acid residue (SAR) containing lead and zinc. A method combining chlorination roasting using CaCl2 with pelletizing for processing SAR containing lead and zinc was used in this study, and the effect of calcium chloride on pelletizing performance was studied; in addition, the removal behavior of lead and zinc was also studied by using polarized light microscopy (Zeiss double Axioskop 40A), X ray diffraction, SEM and EDS. The results showed that CaCl2 migrated to the surface of the pellets during drying, and this phenomenon resulted in a lower removal rate of lead and zinc inside the pellets than outside the pellets during the preheating phase. When the roasting temperature was 1220 °C, with an increase in the basicity of pellets, the silicate minerals in the pellets gradually decomposed, the hematite particles were gradually refined, and more lead or zinc minerals were exposed, which further increased the removal rate of lead and zinc in the pellets. Finally, the SAR pellets with Pb and Zn removal rates up to 91.33 and 97.88%, and a compressive strength of 2789 N, could be obtained, which is very beneficial to the sustainable development of sulfuric acid mills.