As climate change exacerbates water scarcity, rainwater harvesting for household irrigation and gardening becomes an increasingly common practice. However, the use and quality of harvested rainwater are not well studied, and the potential pollutant exposures associated with its use are generally unknown. There are currently no federal standards in the United States to assess metal(loid)s in harvested rainwater. Project Harvest, a community science research project, was created to address this knowledge gap and study the quality of harvested rainwater, primarily used for irrigation, in four environmental justice communities in Arizona, USA. Community scientists collected 577 unique rooftop harvested rainwater samples from 2017 to 2020, which were analyzed for metal(loid)s, where arsenic (As) concentrations ranged from 0.108 to 120 μg L−1 and lead (Pb) concentrations ranged from 0.013 to 350 μg L−1 and compared to relevant federal/state standards/recommendations. Community As and Pb concentrations decreased as: Hayden/Winkelman > Tucson > Globe/Miami > Dewey-Humboldt. Linear mixed models were used to analyze rooftop harvested rainwater data and results indicated that concentrations of As and Pb in the summer monsoon were significantly greater than winter; and contamination was significantly greater closer to extractive industrial sites in three of the four study communities (ASARCO Hayden Plant Superfund Alternative site in Hayden/Winkelman, Davis-Monthan United States Air Force Base in Tucson - Pb only, and Freeport McMoRan Copper and Gold Mine in Globe/Miami). Based on models, infrastructure such as proximity to roadway, roof material, presence of a cistern screen, and first-flush systems were not significant with respect to As and Pb when controlling for relevant spatiotemporal variables; whereas, cistern age was associated with Pb concentrations. These results however, indicate that concentrations vary seasonally and by proximity to industrial activity, not by decisions made regarding collection system infrastructures at the individual home level. This study shows that generally, individuals are not responsible for environmental contamination of rooftop harvested rainwater, rather activities and decisions of government and corporate industries control contaminant release.