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Nanostructured functional oxides play an important role in enabling clean energy technologies and novel memory and processor devices. Using thin‐film La0.6Sr0.4FeO3 (LSF) as a model system, the novel utility of exsolution in fabricating self‐assembled metal oxide nanocomposites with tunable functionalities is shown. Exsolution triggers the formation of metallic iron (Fe0) nanoparticles, Ruddlesden–Popper...