The exploration of a new conceptual strategy for improving the oxygen evolution reaction (OER) of earth-abundant electrocatalysts is critical. In this study, chiral copper oxide nanoflower is explored by a self-assembly method. The characterization suggests the chiral structure originates from the crystal plane-level helical stack of the secondary nanosheets. Of note, the assembly illustrates a record-high degree of spin polarization of 96%, indicating the ideal alignment of electron spin. Moreover, density function theory calculations show the chiral structure reducing the reaction energy barrier (REB) while switching the potential-determining step from *O→*OOH to *OH→*O. Together with the enhanced electrochemical active surface area and accelerated charge transfer, the production of ground-state triplet O2 is improved via a spin-forbidden route that involves the singlet H2O/OH•. Consequently, the chiral nanoflower shows a overpotential of 308mV at 10mA cm-2 and a Tafel slope of 93.5mV dec-1, which is even superior to the commercial RuO2 (310mV, 101mV dec-1). This study presents a new strategy for improving the OER activity by simultaneously enhancing electronic properties and lowering the REB of an non-noble electrocatalyst via chirality engineering.
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