Using mussels as monitoring tools we measured water quality in Sydney Harbour during a large scale, multi-year remediation project of the Sydney Tar Ponds (STPs); one of Canada's most contaminated sites. Chemical contaminants were measured in blue mussels (Mytilus edulis) in Sydney Harbour, which were used as monitoring tools to assess the spatio-temporal distribution of polycyclic aromatic hydrocarbons (PAHs); polychlorinated biphenyls (PCBs); metals (As, Cd, Cu, Hg, Pb, Zn) and lipid content during baseline and 3 years of remediation. The overall spatio-temporal distribution of chemicals in mussels was also compared to contaminants in other marine indicators (e.g., sediment, water and crab tissue). Measured metal concentrations in mussels showed some minor temporal variability (4 years), but these did not appear to be directly related to remediation activities, with the highest concentrations of As, Hg and Zn measured at reference stations. Most measured contaminants showed stable or potentially decreasing concentrations during the study, except Pb and Zn. Individual PAH compounds were mostly undetected during baseline and remediation, except for fluoranthene and pyrene. Concentrations of fluoranthene in mussels and deep water samples were moderately related. Generally, PCBs were undetected (<0.05 μg g(-1)), except during year 2 remediation at some near-field stations. Contaminants measured during this study were at much lower concentrations than previously reported in other studies of mussels in Sydney Harbour and eastern Canada. This is likely due to the ongoing natural recovery of Sydney Harbour and to a lesser extent because of the environmental mitigation protection measures implemented during remediation activities at the STPs. The lack of detection of most individual PAHs and PCBs, plus relatively low bio-accumulation of metals observed during baseline and remediation attest to the effectiveness of using mussels as monitoring tools for environmental quality.