Supplying exogenous sulfur-rich compounds increases the content of glutathione(GSH) and phytochelatins(PCs) in plant tissues, enabling plants to enhance their cellular defense capacity and/or compartmentalize Cadmium(Cd) into vacuoles. However, the mechanism by which surplus S modulates tolerance to Cd stress in different tissues need further investigation. In the present study, we found that supplementing the tartary buckwheat(Fagopyrum tararicum) exposed to Cd with surplus S reversed Cd induced adverse effects, and increased Cd concentrations in roots, but decreased in leaves. Further analysis revealed that exogenous S significantly mitigated Cd-induced oxidative stress with the aids of antioxidant enzymes and agents both in leaves and roots, including peroxidase(POD), ascorbate peroxidase(APX), glutathione peroxidase(GPX), glutathione S-transferase(GST), ascorbic acid(AsA), and GSH, but not superoxide dismutase(SOD) and catalase(CAT). The increased Cd uptake in root vacuoles and decreased translocation in leaves of exogenous S treated plants could be ascribed to the increasing Cd binding on cell walls, chelation and vacuolar sequestration with helps of non-protein thiols(NPT), PCs and heavy metal ATPase 3(FtHMA3) in roots, and inhibiting expression of FtHMA2, a transporter that helps Cd translocation from roots to shoots. Results provide the fundamental information for the application of exogenous S in reversal of heavy metal stress.