The active site for electrocatalytic water oxidation on the highly active iron(Fe)-doped beta-nickel oxyhydroxide (beta-NiOOH) electrocatalyst is hotly debated. Here we characterize the oxygen evolution reaction (OER) activity of an unexplored facet of this material with first-principles quantum mechanics. We show that molecular-like 4-fold-lattice-oxygen coordinated metal sites on the ((1) over bar2 (1) over bar1) surface may very well be the key active sites in the electrocatalysis. The predicted OER overpotential (eta(OER)) for a Fe-centered pathway is reduced by 0.34 V relative to a Ni-centered one, consistent with experiments. We further predict unprecedented, near quantitative lower bounds for the eta(OER), of 0.48 and 0.14 V for pure and Fe doped beta-NiOOH((1) over bar2 (1) over bar1), respectively. Our hybrid density functional theory calculations favor a heretofore unpredicted pathway involving an iron(W)-oxo species, Fe4+=0. We posit that an iron(IV)-oxo intermediate that stably forms under a low coordination environment and the favorable discharge of Ni3+ to Ni2+ are key to beta-NiOOH's OER activity.