Organochlorine pesticides (OCPs) have variously been phased out in agricultural activities, but they are still widely detected in air, water, and soil systems due to their recalcitrant nature in the environment. The purposes of this study were to assess potential OCP pollution via dry and wet deposition over the fast developing Pearl River Delta area with 41,700 km², where the main effort has been focused on emerging pollutants such as petroleum hydrocarbons and PM2.5. We quantified both the dry and wet deposition fluxes of 19 OCPs including dichlorodiphenyltrichloroethanes (DDTs), endosulfans (Endos), and hexachlorocyclohexanes (HCHs). The results showed that each year about 67.4, 42.0, 15.0, and 8.07 kg of total OCPs, DDTs, Endos, and HCHs were returned to the ground, among which 11.7, 10.4, 0.84, and 0.16 kg were in the dry deposition forms. The large spatial variations in OCP deposition fluxes indicated that OCP pollution in the air is mainly influenced on local scales because evaporation from local soil is likely the major source of the phased out OCPs. Source analysis indicated that DDTs may be still in use as antifouling agent and/or dicofol, but Endos and HCHs were mainly derived from the residual of historical usage. The study suggests that the historical OCP pollutants are persistent at high levels in this area and should not be overlooked, while we tackle emerging pollutants.