Trichloroethylene (TCE) is a highly effective industrial degreasing agent and known carcinogen. It was frequently buried improperly in landfills and has subsequently become one of the most common groundwater and soil contaminants in the USA. A common strategy to remediate TCE-contaminated sites and to prevent movement of the TCE plumes into waterways is to construct biowalls which consist of biomaterials and amendments to enhance biodegradation. This approach was chosen to contain a TCE plume emanating from a closed landfill in Maryland. However, predicting the effectiveness of biowalls is often site specific. Therefore, we conducted an extensive series of batch reactor studies at 12 °C as opposed to the typical room temperature to examine biowall fill-material combinations including the effects of zero-valent iron (ZVI) and glycerol amendments. No detectable TCE was observed after several months in the laboratory study when using the unamended 4:3 mulch-to-compost combination. In the constructed biowall, this mixture reduced the upstream TCE concentration by approximately 90% and generated ethylene downstream, an indication of successful reductive dechlorination. However, the more toxic degradation product vinyl chloride (VC) was also detected downstream at levels approximately ten times greater than the maximum contaminant level. This indicates that incomplete degradation also occurred. In the laboratory, ZVI reduced VC formation. A hazard quotient was calculated for the landfill site with and without the biowall. The addition of the biowall decreased the hazard quotient by 88%.