The relationships between metallothionein-like protein (MTLP) and tissue metal (Ni, Cd, Cu, Zn, Pb) concentrations were examined in Oligochaetes and Chironomid larvae collected from reference and metal contaminated sediments. Tissue metal concentrations, for example, Cd reaching 0.3 μmol/g in oligochaetes and Cu, reaching 0.8 μmol/g in chironomids collected from Great Lakes reference sites (Environment Canada) indicated the presence of bioavailable metal at some sites. The concentration of MTLP ranged from 3.3 (± 1.0) to 11.5 (± 4.5) nmol MTLP/g in oligochaetes, and 2.7 (± 1.0) to 8.0 (± 2.7) nmol MTLP/g in chironomids. Individually, tissue metal concentrations were relatively poor (r² = 0.002–0.52) predictors of MTLP, but when multiple metals were used the relationship became stronger (oligochaetes r² = 0.84, p < 0.001; chironomids r² = 0.61, p < 0.001), suggesting that MTLP was induced by multiple metals. Tissue metal and MTLP concentrations in invertebrates from the metal contaminated slips of Collingwood Harbour were not elevated above reference levels, indicating that only a fraction of the metal in the sediment is bioavailable. Chironomids collected from lakes contaminated by atmospheric fallout of smelting emissions (Rouyn-Noranda, QC) had elevated tissue metal concentrations but MTLP concentration did not consistently reflect elevated tissue metal. Overall, MTLP concentrations in invertebrates collected from metal-contaminated sites were not significantly higher than concentrations in reference site-collected invertebrates. The data presented here suggest that, at some sites, MTLP concentration in field-collected organisms would be a useful surrogate for tissue metal but, because of a lack of detailed taxonomy (organisms were designated as chironomids or oligochaetes) and the relatively small sample sizes of this study, no definitive conclusion regarding the suitability of MTLP concentration as a field-based biomarker of metal exposure can be made without further study.