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Layered double hydroxides (LDHs) are among the most active and studied catalysts for the oxygen evolution reaction (OER) in alkaline electrolytes. However, previous studies have generally either focused on a small number of LDHs, applied synthetic routes with limited structural control, or used non-intrinsic activity metrics, thus hampering the construction of consistent structure-activity-relations. Herein, by employing new individually developed synthesis strategies with atomic structural control, we obtained a broad series of crysta