A column study for hexavalent chromium (Cr(VI)) removal from contaminated soil was performed using calcium polysulfide (CPS) and nanoscale zero-valent iron stabilized with green tea extract (GT-nZVI). Injection of CPS at 12 times the stoichiometric requirement (12×) resulted in quantitative Cr(VI) removal for up to 195 days of equivalent groundwater flow. Solid-bound Cr(VI) was reduced up to >99% (<2mg/kg). Treatment with CPS resulted in a short-term release of high sulfur concentrations. Injections of 12× and 24× stoichiometric GT-nZVI resulted in decrease in leachate pH from 6 to 2.5, which rebounded to 4.5 after the equivalent of 45 days and remained stable for the next equivalent 3 years. Metals concentrations in the effluent (Pb, Cr and Fe) increased following injection and quickly decreased, such that the mass flux was low with respect to the total amounts in the solid. Aqueous Cr(VI) was non-detect for the majority of the monitoring time, but concentrations eventually increased with respect to the control sample. Solid-bound Cr(VI) concentrations decreased by 30% and 66% in the 12× and 24× treatments, respectively. The low efficiency was attributed to increased sorption to iron surfaces at pH 2.5 and slow dissolution of PbCrO4, both of which were identified by micro-X-ray fluorescence and absorption analyses.