Iron oxide-bearing minerals have long been recognized as an effective reactive media for arsenic-contaminated groundwater remediation. This research aimed to develop a technique that could facilitate in situ oxidative precipitation of Fe3+ in a soil (sand) media for generating a subsurface iron oxide-based reactive barrier that could immobilize arsenic (As) and other dissolved metals in groundwater. A simple in situ arsenic treatment process was successfully developed for treating contaminated rural groundwater using iron oxide-coated sand (IOCS). Using imbibition flow, the system facilitated the dispersive transport of ferrous iron (Fe2+) and oxidant solutions in porous sand to generate an overlaying blanket where the Fe2+ was oxidized and precipitated onto the surface as ferric oxide. The iron oxide (FeOx) emplacement process was significantly affected by (1) the initial surface area and surface-bound iron content of the sand, (2) the pH and solubility of the coating reagents, (3) the stability of the oxidant solution, and (4) the chemical injection schedule. In contrast to conventional excavate-and-fill treatment technologies, this technique could be used to in situ replace a fresh iron oxide blanket on the sand and rejuvenate its treatment capacity for additional arsenic removal. Several bench-scale experiments revealed that the resultant IOCS could treat arsenic-laden groundwater for extended periods of time before approaching its effective life cycle. The adsorption capacity for As(III) and As(V) was influenced by (1) the amount of iron oxide accumulated on the sand surface, (2) the system pH, and (3) competition for adsorption sites from other groundwater constituents such as silicon (Si) and total dissolved solids (TDS). Although the IOCS could be replenished several times before exhaustion, the life cycle of the FeOx reactive barrier may be limited by the gradual loss of hydraulic conductivity induced by the imminent reduction of pore space over time.