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Chiral-induced spin selectivity is recently demonstrated in a range of spin-dependent optoelectronics and electrochemistry. Herein, a new type of amorphous chiral tartaric acid-FeNi coordination polymer fabricated by electrodeposition methods, achieving both high spin-polarization and high electrocatalytic activity for oxygen evolution, is reported. Circular dichroism shows signature optical activity from the coordination polymer. Conductive atomic force microscopy measurements demonstrate a high spin polarization through the chiral electrocatalyst, which significantly suppresses the formation of hydrogen peroxide byproducts compared to the achiral ones. These chiral Fe-Ni electrocatalysts exhibit a low overpotential of 205 and 280 mV to achieve 10 and 100 mA cm(-2), respectively.