Land use in geographic areas that replenish groundwater and surface water resources is increasingly recognized as an important factor affecting drinking water quality. Efforts to understand the implications for health, particularly outcomes with long latency or critical exposure windows, have been hampered by lack of historical exposure data for unregulated pollutants. This limitation has hindered studies of the possible links between breast cancer risk and drinking water impacted by endocrine disrupting compounds and mammary carcinogens, for example. This paper describes a methodology to assess potential historical exposure to a broad range of chemicals associated with wastewater and land use impacts to 132 groundwater wells and one surface water body supplying drinking water to 18 public distribution systems on Cape Cod, MA. We calculated annual measures of impact to each distribution system and used the measures as exposure estimates for the residential addresses of control women in the Cape Cod Breast Cancer and Environment Study (Cape Cod Study). Impact was assessed using (1) historical chemical measurements of nitrate at the water supply sources (performed as required by the Safe Water Drinking Act) and (2) a geographic information system analysis of land use within the zones of contribution (ZOCs) delineated for each well in a state-mandated wellhead protection program. The period for which these impact estimates were developed was constrained by the availability of chemical measurements and land use data and consideration of time required for groundwater transport of contaminants to the water supply wells. Trends in these estimates for Cape Cod suggest increasing impact to drinking water quality for land use over the study period. Sensitivity analyses were conducted to assess the effect on the distribution of controls' cumulative exposure estimates from (1) reducing the area of the ZOCs to reflect typical well operating conditions rather than extreme pumping conditions used for the regulatory ZOCs, (2) assuming residences received their drinking water entirely from the closest well or cluster of wells rather than a volume-weighted annual district-wide average, and (3) changing the travel time considered for contaminants to reach wells from land use sources. We found that the rank and distribution of controls' cumulative exposure estimates were affected most by the assumption concerning district mixing; in particular, assignment of exposure estimates based on impact values for the closest well(s) consistently produced a larger number of unexposed controls than when a district-wide average impact value was used. As expected, the results suggest that adequate characterization of water quality heterogeneity within water supplies is an important component of exposure assessment methodologies in health studies investigating impacted drinking water.