Many aquatic contaminants, because of low water solubility (hydrophobicity) or association with floatable particles, concentrate at the sea surface. Thirty-six samples of the sea-surface microlayer (SMIC), the upper 50 μm, were collected from sites in Puget Sound, Washington State. Sites included three urban bays, central Puget Sound, and a rural reference site. Exposure of floating fish eggs to approximately half of these samples resulted in sublethal and lethal toxic effects (Hardy et al., 1987c). Chemical analyses revealed high concentrations of contaminants in many of the samples. Major temporal and spatial differences in sea-surface chemistry occurred, but maximum (for all) and mean (for 1985) concentrations were aromatic hydrocarbons, 8030 (mean 132) μg liter −1: saturate hydrocarbons, 2060 μg liter −1: pesticides, 43·8 (mean 0·46) ng liter −1; PCBs, 3890 (mean 631) ng liter −1; and total metals, 4750 (mean 626) μg liter −1. Stepwise multivariate regression indicated that the percentage of fish eggs developing to normal live larvae decreased with increasing concentrations of a complex mixture of contaminants. Principal component analysis demonstrated that the major types of contaminants did not differ greatly in their statistical contribution to the toxicity, i.e. no single chemical was responsible for the observed toxicity. The chemical composition of the SMIC samples suggested that contamination originated from a variety of sources including atmospheric deposition, terrestrial runoff of fossil fuel combustion products, and sewage disposal.