The residues and enantiomeric fractions of organochlorine pesticides (OCPs) were measured in 11 mollusk species collected from the coastal areas along the Yangtze River Delta to evaluate the status, potential sources, and health risks of pollution in these areas. The concentrations of DDTs, HCHs, and chlordanes ranged from 6.22 to 398.19, 0.66–7.11, and 0.14–4.08ngg−1 based on wet weight, respectively; DDTs and HCHs have the highest values, globally. The DDTs increased and the HCHs decreased compared to historical data. Both the box-and-whisker plots and the one-way ANOVA tests indicated that the OCP levels varied little between sampling locations and organism species. The compositions of the DDTs and HCHs suggested a cocktail input pattern of fresh and weathered technical products. The comparative EF values for the α-HCH between the sediments and mollusks, as well as the lack of any discernible difference in the relative proportions of HCH isomers among different species from the same sampling site implied that the HCH residues in the mollusks came directly from the surrounding environment. However, the biotransformation of DDTs in mollusks cannot be precluded. The assessments performed based on several available guidelines suggested that although no significant human health risks were associated with the dietary intake of OCPs, the concentrations of DDTs exceeded the maximum residual limits of China and many developed nations. Moreover, an increased lifetime cancer risk from dietary exposure to either DDTs or HCHs remains a possibility. Because non-racemic OCP residues are common in the mollusk samples, our results suggest a need to further explore the levels and toxicity of the chiral contaminants in mollusks and other foodstuff to develop the human risk assessment framework based on chiral signatures.