This article is the first in a series of three that describe the results of a Natural Resource Damage Assessment (NRDA) conducted in the Grand Calumet River and Indiana Harbor Area of Concern (IHAOC). The assessment area is located in northwest Indiana and was divided into nine reaches to facilitate the assessment. This component of the NRDA was undertaken to determine if sediments and sediment-dwelling organisms have been injured due to exposure to contaminants that have accumulated in sediments as a result of discharges of oil or releases of other hazardous substances from industrial, municipal, and nonpoint sources. To support this assessment, information was compiled on the chemical composition of sediment and pore water; on the toxicity of whole sediments, pore water, and elutriates; and on the status of benthic invertebrate communities. The data on each of these indicators were compared to regionally relevant benchmarks to assess the presence and extent of injury to surface water resources (i.e., sediments) or biological resources (i.e., sediment-dwelling organisms). The results of this assessment indicate that sediment injury has occurred throughout the assessment area, with up to four distinct lines of evidence demonstrating injury within the various reaches. The primary contaminants of concern (i.e., those substances that are present at concentrations that are sufficient to cause or substantially contribute to sediment injury) include metals, polycyclic aromatic hydrocarbons, and total polychlorinated biphenyls.