Pollutant data for air, water, soil and biota were compiled from databases and internet sources and by staff interviews at 23 National Park Service (NPS) units in 2005. A metric was derived describing the quality and quantity of data for each park, and in combination with known contaminant threats, the need for ecotoxicological study was identified and ranked. Over half of NP units were near Toxic Release Inventory sites discharging persistent pollutants, and fish consumption advisories were in effect at or near 22 of the units. Pesticide and herbicide use was found to be minimal, with the exception of those units with agricultural leases. Only 70 reports were found that describe terrestrial vertebrate environmental contaminant data at or near the units. Of the >75,000 compounds in commerce, empirical exposure data were limited to merely 58 halogenated compounds, insecticides, rodenticides, metals, and some contemporary compounds. Further ecotoxicological monitoring and research is warranted at several units including Shenandoah National Park, Richmond National Battlefield Park, Chesapeake & Ohio Canal National Historical Park, Valley Forge National Historical Park, Hopewell Furnace National Historic Site, Monocacy National Battlefield, and Harpers Ferry National Historical Park. The types of investigations vary according to the wildlife species present and potential contaminant threats, but should focus on contemporary use pesticides and herbicides, polychlorinated biphenyls, mercury, lead, and perhaps antibiotics, flame retardants, pharmaceuticals, and surfactants. Other management recommendations include inclusion of screening level contaminant risk assessments into the NPS Vital Signs Program, development of protocols for toxicological analysis of seemingly affected wildlife, alternative methods and compounds for pest management, and use of non-toxic fishing tackle by visitors.