Even though the application of dichlorodiphenyltrichloroethanes (DDTs) has been restricted for over 30 years, their ubiquitous existence still poses profound adverse impacts on ecosystem and human health. In this study, simultaneous soil and air sampling campaigns at different functional areas were conducted in warm and cold seasons. Based on the residue levels and enantiomeric signatures of DDT and its metabolites in soils and air, the parameters influencing ecological and human health risks were explored. Sigma DDT concentrations in soils correlated positively with organic matter (OM) and negatively with pH, whereas atmospheric DDT levels were primarily facilitated by increased temperature. High temperature and low soil pH were also favorable for the transformation of DDT into its metabolites. The inhabitants living in agricultural regions or in areas with higher soil OM or pH < 7 were exposed to higher existing and potential health risks of soil DDTs. In addition, at lower temperatures, the existing and potential carcinogenic risks of DDTs from soil exposure were higher, whereas risks from air inhalation were lower. Health risks would be increased when considering the enantioselective toxicity of o,p'-DDT and o,p'-DDD. The results from this study could provide baseline support for risk control and avoidance of DDTs.