摘要：Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic ***,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water ***,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)*** measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band ***,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C *** work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.