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Metallic iron (Fe⁰) corrosion under immersed conditions (Fe⁰/H₂O system) has been used for water treatment for the past 170 years. Fe⁰ generates solid iron corrosion products (FeCPs) which are known to in situ coat the surface of aggregates, including granular activated carbon (GAC), gravel, lapillus, manganese oxide (MnO₂), pyrite (FeS₂), and sand. While admixing Fe⁰ and reactive aggregates to build hybrid systems (e.g., Fe⁰/FeS₂, Fe⁰/MnO₂, Fe⁰/sand) for water treatment, it has been largely overlooked that these materials would experience reactivity loss upon coating. This communication clarifies the relationships between aggregate addition and the sustainability of Fe⁰/H₂O filtration systems. It is shown that any enhanced contaminant removal efficiency in Fe⁰/aggregate/H₂O systems relative to the Fe⁰/H₂O system is related to the avoidance/delay of particle cementation by virtue of the non-expansive nature of the aggregates. The argument that aggregate addition sustains any reductive transformation of contaminants mediated by electrons from Fe⁰ is disproved by the evidence that Fe⁰/sand systems are equally more efficient than pure Fe⁰ systems. This demonstration corroborates the concept that aqueous contaminant removal in iron/water systems is not a process mediated by electrons from Fe⁰. This communication reiterates that only hybrid Fe⁰/H₂O filtration systems are sustainable.