Studies were undertaken to determine the reasons why published information regarding the efficiency of metallic iron (Fe0) for water treatment is conflicting and even confusing. The reactivity of eight Fe0 materials was characterized by Fe dissolution in a dilute solution of ethylenediaminetetraacetate (Na2–EDTA; 2 mM). Both batch (4 days) and column (100 days) experiments were used. A total of 30 different systems were characterized for the extent of Fe release in EDTA. The effects of Fe0 type (granular iron, iron nails and steel wool) and pretreatment procedure (socking in acetone, EDTA, H2O, HCl and NaCl for 17 h) were assessed. The results roughly show an increased iron dissolution with increasing reactive sites (decreasing particle size: wool > filings > nails), but there were large differences between materials from the same group. The main output of this work is that available results are hardly comparable as they were achieved under very different experimental conditions. A conceptual framework is presented for future research directed towards a more processed understanding.