Pertechnetate oxyanion (TcO4-), which is highly soluble in water and readily mobile in the environment, can be immobilized through an ion exchange/adsorption process and chemical reduction followed by adsorption and/or precipitation. Previous studies have focused on the separation and removal of (TcO4-)-Tc-99 from high-level waste streams; however, little information is available for (TcO4-)-Tc-99 removal from only slightly contaminated groundwater. This paper describes treatment of (TcO4-)-Tc-99-contaminated groundwater with both batch and column flowthrough experiments. Synthetic resins and sponges, and zero-valence iron filings were used to evaluate their capacities and the rates of (TcO4-)-Tc-99 removal. The toxicity characteristic leaching procedure (TCLP) was applied to evaluate the leachability of Tc-99 adsorbed or co-precipitated on iron. Results suggest that both iron and synthetic resins remove (TcO4-)-Tc-99 from groundwater and that at a high flow rate (with residence time of less than 1 min), (TcO4-)-Tc-99 removal capacity is greater for iron filings than for the synthetic resins on a volume basis. Additionally, the rate of (TcO4-)-Tc-99 sorption on the sponge is slow (approximately 3 days), and the capacity is relatively low. No appreciable amount of Tc-99 can be leached out from the spent iron filings by the TCLP test. Overall, zero-valence iron filings provide fast reaction and high removal capacity for (TcO4-)-Tc-99 in groundwater. The high removal efficiency, low cost, and the small waste production of zero-valence iron are attractive for remediation of (TcO4-)-Tc-99-contaminated groundwater.