Efforts to achieve the decomposition of carbon tetrachloride through anaerobic and aerobic bioremediation and chemical transformation have met with limited success because of the conditions required and the formation of hazardous intermediates. Recently, particles of zero-valent iron (ZVI) have been used with limited success for in situ remediation of carbon tetrachloride. We studied a modified microparticulate product that combines controlled-release carbon with ZVI for stimulation of in situ chemical reduction of persistent organic compounds in groundwater. With this product, a number of physical, chemical, and microbiological processes were combined to create very strongly reducing conditions that stimulate rapid, complete dechlorination of organic solvents. In principle, the organic component of ZVI microparticles is nutrient rich and hydrophilic and has high surface area capable of supporting the growth of bacteria in the groundwater environment. In our experiments, we found that as the bacteria grew, oxygen was consumed, and the redox potential decreased to values reaching −600 mV. The small modified ZVI particles provide substantial reactive surface area that, in these conditions, directly stimulates chemical dechlorination and cleanup of the contaminated area without accumulation of undesirable breakdown products. The objective of this work was to evaluate the effectiveness of ZVI microparticles in reducing carbon tetrachloride under laboratory and field conditions. Changes in concentrations and in chemical and physical parameters were monitored to determine the role of the organic products in the reductive dechlorination reaction. Laboratory and field studies are presented.