Chemical contaminants were assessed in Sydney Harbour, Nova Scotia during pre-remediation (baseline) and 3 years of remediation of a former coking and steel facility after nearly a century of operation and historical pollution into the Sydney Tar Ponds (STP). Concentrations of polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls, metals, and inorganic parameters measured in sediments and total suspended solids in seawater indicate that the overall spatial distribution pattern of historical contaminants remains unchanged, although at much lower concentrations than previously reported due to natural sediment recovery, despite remediation activities. Measured sediment deposition rates in bottom-moored traps during baseline were low (0.4-0.8 cm year(-1)), but during dredging operations required for construction of new port facilities in the inner Sydney Harbour, sedimentation rates were equivalent to 26-128 cm year(-1). Measurements of sediment chemical contaminants confirmed that natural recovery rates of Sydney Harbour sediments were in broad agreement with predicted concentrations, or in some cases, lower than originally predicted despite remediation activities at the STP site. Overall, most measured contaminants in sediments showed little temporal variability (4 years), except for the detection of significant increases in total PAH concentrations during the onset of remediation monitoring compared to baseline. This slight increase represents only a short-term interruption in the overall natural recovery of sediments in Sydney Harbour, which were enhanced due to the positive impacts of large-scale dredging of less contaminated outer harbor sediments which were discharged into a confined disposal area located in the inner harbor.