The release of a 14C-labeled trichlorobiphenyl compound ([14C]PCB 32) from sediment to water was quantified weekly in a 30-d microcosm experiment with recirculating water. Two modes of bioturbation-driven polychlorinated biphenyl (PCB) release—bioturbation by the amphipod Monoporeia affinis (a particle biodiffuser) and bioturbation by the polychaete Marenzelleria sp. (a bioirrigator)—were compared to the PCB release caused by physical resuspension of the sediment generated by a motor-driven paddle used twice a week. Bioturbation by the amphipod M. affinis caused a significantly higher remobilization of both particle-associated PCB (PCBpart) and dissolved PCB (PCBdiss) than the other treatments. Bioturbation by Marenzelleria sp. and physical resuspension caused a similar release of PCBdiss despite a significantly higher amount of total suspended solids in the water column after physical resuspension. In all treatments, the release of PCBdiss was more than one order of magnitude higher than that of PCBpart, indicating a significant potential route of exposure for pelagic organisms, such as fish, to the most bioavailable PCB form. Calculated mass-transfer coefficients (0.3–1.3 cm/d) correspond to previously reported values for trichlorinated PCBs. The present results indicate that biological reworking of sediments can be just as, or even more, important than physical resuspension for the remobilization of sediment-bound contaminants.