Surface water quality closely correlating with human health suffered increasing organochlorine pesticide (OCP) pollution due to the intensive anthropogenic activities in megacities. In the present study, 112 water samples collected from 14 lakes and 11 drinking water source sites inWuhan were detected for the residues of OCPs in November 2013 and July 2014, respectively. The ΣOCPs ranged from 5.61 to 13.62 ng L−1 in summer with the maximum value in Yezhi Lake and 3.18 to 7.73 ng L−1 in winter with the highest concentration in Yandong Lake. Except dichlorodiphenyltrichloroethanes (DDTs), OCP concentrations in summer were significantly higher than those in winter mostly due to the nonpoint source pollution including land runoff in summer. Source apportionment of hexachlorocyclohexanes (HCHs) and DDTs revealed the historical use of technical HCH and lindane and the new input of DDT, respectively. The spatial distribution of OCPs was not uniform in the surface water of Wuhan because of the significant influence of land development and fishery. The risk assessments showed the heptachlor, and heptachlor epoxide in most sampling sites exceeded the threshold set by the European Union, indicating the possible adverse effects for aquatic lives. Negligible non-carcinogenic risks for drinking and bathing as well as carcinogenic risks for bathing were found in the surface water. However, the total carcinogenic risks of all OCPs (ΣRs) caused by drinking in summer were higher than the safe level of 10−7 in all sampling sites. It was implied that the surface water in Wuhan was not safe for directly drinking without effective purification.