LAUSR

Despite the increasing effort in advancing oxygen electrocatalysts for zinc‐air batteries (ZABs), the performance development gradually reaches a plateau via only ameliorating the electrocatalyst materials. Herein, a new class of external field‐responsive electrocatalyst comprising Ni0.5Mn0.5Fe2O4 stably dispersed on N‐doped Ketjenblack (Ni0.5Mn0.5Fe2O4/N‐KB) is developed via polymer‐assisted strategy for practical ZABs. Briefly, the activity indicator ΔE is significantly decreased to 0.618 V upon photothermal assistance, far exceeding most reported electrocatalysts (generally >0.680 V). As a result, the photothermal electrocatalyst possesses comprehensive merits of excellent power density (319 mW cm−2), ultralong lifespan (5163 cycles at 25 mA cm−2), and outstanding rate performance (100 mA cm−2) for liquid ZABs, and superb temperature and deformation adaptability for flexible ZABs. Such improvement is attributed to the photothermal‐heating‐enabled synergy of promoted electrical conductivity, reactant‐molecule motion, active area, and surface reconstruction, as revealed by operando Raman and simulation. The findings open vast possibilities toward more‐energy‐efficient energy applications.