This dissertation combines field data, laboratory experiments, and mathematic models to (1) predict the probability of groundwater arsenic (As) contamination caused by geogenic sources and processes in shallow aquifers of the Mississippi Delta in southern Louisiana, (2) study the role microbes play in controlling As mobilization from sediments to groundwaters, and (3) simulate As mobilization and transport caused by changing redox conditions and groundwater geochemistry along a flow path within the southeastern Chicot aquifer in southern Louisiana. A model based on surface hydrology, soil properties, geology, and sedimentary deposition environments predicts that the Holocene shallow aquifers in southern Louisiana are at high risk of As contamination. Sediment incubation and pore-water chemistry suggest that microbes play a key role in mobilizing As from sediments by reductive dissolution of As-bearing Fe(III) oxides/oxyhydroxides. Finally, groundwater samples were collected along a 10 km flow path in the southeastern Chicot aquifer to determine groundwater geochemical parameters and to simulate reactive transport of Fe and As species along the studied flow path. The model well captures the general trends of Fe(II) and As(III) concentrations along the studied flow path and the close correspondence between Fe(II) and As(III) of the both measured and model predicted As(III) and Fe(II) concentrations support the hypothesis that microbially mediated reductive dissolution of As-bearing Fe(III) oxides/oxyhydroxides is the primary mechanism causing As mobilization from sediments to the shallow reducing groundwaters of the Mississippi Delta in southern Louisiana. / 1 / NINGFANG YANG