The fabrication of an economical, earth-abundant, environment-friendly, and highly efficient electrocatalyst for anodic oxygen evolution reaction (OER) in the electrolysis of water is essential for sustainable energy conversion and storage technology. Among the various transition metal-based electrocatalysts, iron-based electrocatalysts are well-known for their catalytic behavior due to their effective redox activity, abundance, and low toxicity. Pyrites are the most prevalent Fe-containing minerals in the earth's crust, but their use as an electrocatalyst for oxygen evolution reaction (OER) has received little attention though their synthetic counterparts have shown better activity. Herein, the naturally occurring pyrite (FeS2) on Ni foam is evaluated as a dynamic electrocatalyst towards OER in alkaline media. Various spectro-analytical techniques have been used to confirm the chemical and physical characteristics of earth abundant pyrite. The pyrite-coated nickel foam exhibited an extraordinarily superior catalytic activity for OER with overpotential of 203 and 315 mV at current densities of 10 mA∙cm−2 and 50 mA∙cm−2, respectively in 1.0 M potassium hydroxide (KOH) electrolyte at a scan rate of 5 mV∙s−1. Meanwhile, the benchmark precious iridium oxide (IrO2) on nickel foam demonstrated an overpotential of 322 and 430 mV for OER at 10 and 50 mA∙cm−2, respectively. It's important to note that the catalyst used is a natural pyrite with some additional constituents in small quantities. Therefore, the analysis revealed the presence of carbon (C), silicon (Si) and oxygen (O) in addition to FeS2. This composition, along with the synergistic behavior of nickel ions from the nickel foam, likely contributes to the enhancement in catalytic activity observed. The pyrite on carbon substrate, did not exhibit the same impressive OER activity as like on Ni foam, emphasizing the significance of the substrate-dependent performance. Nevertheless, on the nickel foam, natural pyrite displayed the lowest overpotential, Tafel slope, and better stability for OER. Hence, on Ni foam substrate, earth-abundant, low-cost, stable, and efficient pyrite-based catalyst augmented by synergistic interactions with nickel ions, may hold great promise for advancing the field of water electrolysis and facilitating cleaner energy production and conversion.