Polycyclic aromatic hydrocarbon (PAHs) and polychlorinated biphenyls (PCBs) accumulated by semipermeable membrane device (SPMD)-based virtual organisms (VOs) and local feral fish were studied in Three Gorges Reservoir (TGR), China. VOs were deployed at seven sites in TGR for two periods in 2009 and 5 species of fish with different living habitats and feeding habits collected in the same periods from two counties in TGR. The concentration and profile of PAHs and PCBs in fish were quite different fromthose in VOs. Most high-molecular-weight-PAHswere detected in VOs, while theywere undetected in fish.Most PCBs were undetected inVOs,whilemost of them were detected in fish. Low-molecular-weight-PAHs were predominant contaminants of PAHs and nondioxin-like-PCBs were the main PCBs in fish. The levels of PAHs and PCBs in the few fish samples were low and were not of concern based on chemical contaminant limits of non-carcinogenic effect.