DDTs were detected in yellowfin tuna (Thunnus albacares, 92.1–221.8 ng‧g−1 lipid weight) and their prey (54.9–93.5 ng‧g−1 lipid weight) from the South China Sea (SCS). DDT levels reported in this study were lower than those of the previous studies indicated the recent mitigation of DDT contamination in the SCS. Higher DDT levels were observed in fat abdominal muscle than lean dorsal muscle in adult yellowfin tuna. Meanwhile, DDT levels in adult yellowfin tuna were higher than the young ones. The composition profiles of DDT and its metabolites suggested DDTs in fish in the SCS were mainly derived from the historical use of technical DDTs. DDTs were biomagnified through food chains with the trophic magnification factor of 2.5. Risk assessment results indicated that dietary exposure to DDTs through lifetime fish consumption from the SCS would pose little cancer and noncarcinogenic risk to coastal residents.