Correlation analyses between measures of toxicity and concentrations of chemical contaminants were conducted for 103 surficial sediments from Sydney Harbour, Australia, and vicinity. Toxicity tests consisted of amphipod survival and reburial tests of whole sediments (Corophium colo), sea urchin fertilisation and larval development tests of pore waters (Heliocidaris tuberculata) and microbial bioluminescence (Microtox) tests of solvent extracts and pore waters. Toxicity in most tests correlated with concentrations of metallic contaminants, in particular, zinc, lead and copper. Organic contaminants did not correlate as significantly with toxicity. However, Heliocidaris tuberculata showed relationships with organochlorine compounds in samples with low to moderate metals contamination. Toxicity in the Microtox solvent extract test appeared to be primarily influenced by the presence of sulfur. This study has no precedent in Australia and the results support the validity of using local indigenous species in toxicity tests of field-collected sediments. This toxicity/chemistry dataset may be used in evaluations of sediment quality guidelines recently introduced to Australia.