Arsenic in groundwater in excess of the drinking water limit is usually from natural sources. The release of As, however, can be amplified by anthropogenic inputs of carbon, including those associated with the remediation of chlorinated solvents such as trichloroethylene (TCE). Large laboratory columns (15.2 cm diameter, 183 cm long) packed with aquifer solids from a TCE contaminated site near Hill Air Force Base (Utah) were fed with groundwater containing TCE and were biostimulated, bioaugmented, and monitored for TCE dechlorination over 7.5 years. This is a basin‐fill aquifer with As bearing geologic features. The objective of this study was to evaluate the biogeochemical changes that affect As solubilization that occurred after 7.5 years of feeding the columns with either whey or two formulations of Newman Zone® emulsified oil, and a no carbon addition control. The columns were analyzed in 10.16 cm sections for pore water and sediment quality parameters, parameters descriptive of redox conditions, and As geochemistry. The whey treatment resulted in 52.9% (±1.36%) (average ± standard deviation) of the total As in the solids leaching from the columns. The oil treatments promoted loss of 20.9% (±6.40%) of the total As. Arsenic solubility was associated with strongly reducing conditions developed with whey addition, leading to dissolution of crystalline Fe oxides and release of As. Arsenic was attenuated within the oil treated columns with As associated with carbonates in the lower layers. A consequence of adding whey, resulting in the desired full dechlorination of TCE in this aquifer, is the mobilization of As in groundwater.