Nanosized zerovalent iron (NZVI) Fe@Fe 3 O 4 with a core−shell structure derived from photocatalytic MeOH aqueous solution of dinitrosyl iron complex (DNIC) eosin Y, and triethylamine (TEA) is demonstrated. The NZVI Fe@Fe 3 O 4 core shows a high percentage of zerovalent iron (Fe 0 %) and is stabilized by a hydrophobic organic support formed through the photodegradation of eosin Y hybridized with the N 3 MDA ligand. In addition to its well-known reductive properties in wastewater treatment and groundwater remediation, NZVI demonstrates the ability to form heterostructures when it interacts with metal ions. In this research, Co 2+ is employed as a model contaminant and reacted with NZVI Fe@Fe 3 O 4 to result in the formation of a distinct Fe−Co heterostructure, cracked NZVI (CNZVI). The slight difference in the standard redox potentials between Fe 2+ and Co 2+ , the magnetic properties of Co 2+ , and the absence of surface hydroxides of Fe@Fe 3 O 4 enable NZVI to mildly reduce Co 2+ and facilitate Co 2+ penetration into the iron core. Taking advantage of the well-dispersed nature of CNZVI on an organic support, the reduction in particle size due to Co 2+ penetration, and Fe−Co synergism, CNZVI is employed as a catalyst in the alkaline oxygen evolution reaction (OER). Remarkably, CNZVI exhibits a highly efficient OER performance, surpassing the benchmark IrO 2 catalyst. These findings show the potential of using NZVI as a template for synthesizing highly efficient OER catalysts. Moreover, the study demonstrates the possibility of repurposing waste materials from water treatment as valuable resources for catalytic energy conversion, particularly in water oxidation processes.