With the ending of the Cold War, the US and other nations were faced with a legacy of nuclear wastes. For some sites where hazardous nuclear wastes will remain in place, methods must be developed to protect human health and the environment. Biomonitoring is one method of assessing the status and trends of potential radionuclide exposure from nuclear waste sites, and of providing the public with early warning of any potential harmful exposure. Amchitka Island (51 degrees N lat, 179 degrees E long) was the site of three underground nuclear tests from 1965 to 1971. Following a substantive study of radionuclide levels in biota from the marine environment around Amchitka and a reference site, we developed a suite of bioindicators (with suggested isotopes) that can serve as a model for other sites contaminated with radionuclides. Although the species selection was site-specific, the methods can provide a framework for other sites. We selected bioindicators using five criteria: (1) occurrence at all three test shots (and reference site), (2) receptor groups (subsistence foods, commercial species, and food chain nodes), (3) species groups (plants, invertebrates, fish, and birds), (4) trophic levels, and (5) an accumulator of one or several radionuclides. Our major objective was to identify bioindicators that could serve for both human health and the ecosystem, and were abundant enough to collect adjacent to the three test sites and at the reference site. Site-specific information on both biota availability and isotope levels was essential in the final selection of bioindicators. Actinides bioaccumulated in algae and invertebrates, while radiocesium accumulated in higher trophic level birds and fish. Thus, unlike biomonitoring schemes developed for heavy metals or other contaminants, top-level predators are not sufficient to evaluate potential radionuclide exposure at Amchitka. The process described in this paper resulted in the selection of Fucus, Alaria fistulosa, blue mussel (Mytilus trossulus), dolly varden (Salvelinus malma), black rockfish (Sebastes melanops), Pacific cod (Gadus macrocephalus), Pacific halibut (Hippoglossus stenolepis), and glaucous-winged gull (Larus glaucescens) as bioindicators. This combination of species included mainly subsistence foods, commercial fish, and nodes on different food chains.