Mercury (Hg) contamination in soils is of concern because of its known adverse effects on ecosystem functions and human health. Research on how to reduce Hg contamination in soil is still needed, mainly because of the difficulties in remediating Hg-contaminated soils while minimizing adverse effects on treated systems. We investigated the potential of a waste substrate, aluminum (Al)-based drinking water treatment residuals (Al-WTRs), as a low-cost sorbent for immobilizing the mobile fraction of Hg in contaminated soils using column leaching studies. Because of the known role of acidic deposition and dissolved organic matter on the environmental cycling of Hg, columns packed with Hg-contaminated alluvial soils collected from the watershed of Poplar Creek in Tennessee of USA were leached using either the synthetic precipitation leaching procedure (SPLP) to simulate the effects of acid rain or low pH dissolved organic carbon (DOC) rich river water (Suwannee River water, pH 4.20) to mimic soil flooding events with DOC-rich waters. The results show that, for soils with very high mobile Hg fractions, control columns without Al-WTR leached with the SPLP solution retained only 51% of total-Hg, which was significantly less (p < 0.05) than in the Al-WTR treated soil columns (up to 80%). Leaching with DOC-rich river water (53.3 mg C/L) decreased the sorption capacity of Al-WTR. Using waters with increasing DOC concentrations (from 5.33 to 40 mg C/L) resulted in the removal of 63% of the initial mass of Hg in the control columns compared to 22–29% in the columns amended with 2 and 5% Al-WTR. Overall, Al-WTR can immobilize Hg under extreme leachability conditions and should be considered as a potential sorbent for in situ remediation of Hg-contaminated soils. However, further studies are needed on the fate of Al-WTR-immobilized Hg.