Soil lead (Pb) and arsenic (As) are the two highest priority contaminants on the ATSDR-EPA Substance Priority List representing significant toxicity and occurrence at Superfund sites. Neurodevelopmental ramifications of childhood Pb exposure, especially for those ≤ 5 years of age, cause permanent losses in IQ, resulting in approximately 824 million IQ points lost in the United States during the last century. Additionally, As is a widespread carcinogen. Despite the severity, soil remediation methods are largely limited to resource intensive soil removal and replacement strategies. In response, EPA ORD has recently developed a potential in situ solution: conversion of soil Pb and As to jarosite family minerals. Plumbojarosite (PLJ) is a naturally occurring mineral that has low solubility at acidic conditions, resulting in PLJ being exceptionally effective at limiting the soluble Pb fraction that is available for transport across the gastrointestinal barrier and absorption into systemic circulation (i.e., bioavailability). Here, we showcase the progression of jarosite-based remediation methods over the past 6 years for more than 50 soil treatments. For all soil treatments, Pb and As bioaccessibility commonly decreased by >70% whereas the highest efficiency methods have been found to decrease Pb and/or As bioaccessibility and relative bioavailability to <5%. Recent investigations have focused on refining methodology to facilitate field implementation that are actively being planned with support from the EPA Office of Land and Emergency Management. Ultimately, the proposed methods have the potential to drastically decrease soil remediation costs while providing exceedingly effective Pb and As exposure mitigation.