Arsenic (As), a known carcinogen, is a groundwater contaminant in many parts of the world. Arsenic contamination is enhanced through carbon addition, such as biostimulation, a remediation process, which has been used to remove trichloroethylene (TCE) from sediment and groundwater. Two studies were designed to evaluate the effect of different carbon sources on the removal of TCE through dechlorination and on As solubilization and mobilization in response to carbon addition. The first set of columns (15.2 cm diameter, 183 cm long) used whey, Newman Zone® standard surfactant emulsified oil, Newman Zone® nonionic surfactant emulsified oil, and no carbon controls as carbon and energy sources and were fed for 7.5 years. The second set (7.62 cm diameter and length) used whey, lactate, and no carbon control as carbon sources with columns being dismantled and analyzed over a 5-month time period. These studies showed that reducing conditions, caused by the carbon sources, was the driving force for As mobilization as As(V) was reduced to the more mobile As(III). Total As mass in the sediment was lost with all carbon treatments within the first study with whey having a greater loss; however, within the second study, both whey and lactate treatments had the same extent of As mass loss over time. The results also indicated that some As could be attenuating with carbonates or other highly soluble minerals.