Electricity generation and chemical productions are both critically important for the sustainable development of modern civilization. Here, a novel bifunctional Zn‐organic battery has been established for the concurrent enhanced electricity output and semi‐hydrogenations of a series of biomass aldehyderivatives, for the high value‐added chemical syntheses. Among them, the typical Zn‐furfural (FF) battery equipped with Cu foil‐supported edge‐enriched Cu nanosheets as cathodic electrocatalyst (Cu NS/Cu foil), provides a maximum current density and power density of 14.6 mA cm−2 and 2.00 mW cm−2, respectively, and in the meantime, produces high value product, furfural alcohol (FAL). The Cu NS/Cu foil catalyst exhibits excellent electrocatalytic performance of ≈93.5 % conversion ratio and ≈93.1 % selectivity for FF semi‐hydrogenation at a low potential of ‐1.1 V vs. Ag/AgCl by using H2O as H source, and shows impressive performance for various biomass aldehyderivatives semi‐hydrogenation.