Acidic groundwater generated from pyrite oxidation in acid sulfate (AS) soil is a major geoenvironmental problem in Australia. This study aims to evaluate recycled concrete as a reactive material in permeable reactive barriers (PRBs) for the remediation of acidic groundwater in low-lying AS soil floodplains. Laboratory experiments were systematically conducted to investigate the acid neutralization behavior of recycled concrete and its potential to remove dissolved Al and Fe. The results confirmed that recycled concrete could effectively treat acidic groundwater from an AS soil terrain, resulting in near neutral effluent over a long period with complete removal of Al and Fe. The major mechanisms involved in neutralizing acidic groundwater are thought to be the precipitation of Al and Fe as oxides, oxyhydroxides, and hydroxides. However, the accumulation of secondary minerals could decrease the reactivity of the recycled concrete. For example, chemical armoring could decrease the neutralizing capacity of recycled concrete by up to 50% compared with the theoretical acid neutralization capacity of this material. The results reported here also show that the neutralization capacity and reactive efficiency of recycled concrete are dependent on the initial pH value and also the concentration of Al and Fe in acidic groundwater.