The Contaminant Exposure and Effects—Terrestrial Vertebrates (CEE-TV) database was developed to conduct simple searches for ecotoxicological information, examine exposure trends, and identify significant data gaps. The CEE-TV database contains 16,696 data records on free-ranging amphibians, reptiles, birds, and mammals residing in estuarine and coastal habitats of the Atlantic, Gulf, and Pacific coasts, Alaska, Hawaii, and the Great Lakes. Information in the database was derived from over 1800 source documents, representing 483 unique species (about 252,000 individuals), with sample collection dates spanning from 1884 to 2003. The majority of the records contain exposure data (generally contaminant concentrations) on a limited number (n = 209) of chlorinated and brominated compounds, cholinesterase-inhibiting pesticides, economic poisons, metals, and petroleum hydrocarbons, whereas only 9.3% of the records contain biomarker or bioindicator effects data. Temporal examination of exposure data provides evidence of declining concentrations of certain organochlorine pesticides in some avian species (e.g., ospreys, Pandion haliaetus), and an apparent increase in the detection and possibly the incidence of avian die-offs related to cholinesterase-inhibiting pesticides. To identify spatial data gaps, 11,360 database records with specific sampling locations were combined with the boundaries of coastal watersheds, and National Wildlife Refuge and National Park units. Terrestrial vertebrate ecotoxicological data were lacking in 41.9% of 464 coastal watersheds in the continental United States. Recent (1990–2003) terrestrial vertebrate contaminant exposure or effects data were available for only about half of the National Wildlife Refuge and National Park units in the geographic area encompassed by the database. When these data gaps were overlaid on watersheds exhibiting serious water quality problems and/or high vulnerability to pollution, 72 coastal watersheds, and 76 National Wildlife Refuge and 59 National Park units in the continental United States were found to lack recent terrestrial vertebrate ecotoxicology data. Delineation of data gaps in watersheds of concern can help prioritize monitoring in areas with impaired water quality and emphasize the need for comprehensive monitoring to gain a more complete understanding of coastal ecosystem health.