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[Display omitted] • Ni-Co alloy nanoparticles were induced to grow on layered perovskite. • The cell renders 1.53A cm−2 at 2.0 V and 850 °C for CO 2 electrolysis. • Faradic efficiencies of the SOEC are higher than 90 % above 1.6 V. • No degradation was observed in a stability test for 32 h. It has never been more important to develop new technologies that can reduce CO 2 emissions or convert them into useful chemical products. As solid-state electrochemical devices, solid oxide electrolysis cell (SOEC) is capable of converting CO 2 efficiently and selectively into CO or, when combined with water electrolysis, producing syngas (CO and H 2). Herein, we demonstrate a novel layered perovskite oxide, reduced (La 4 Sr 4) 0.9 Ti 7.2 Ni 0.4 Co 0.4 O 26 (LSTNC-r), decorated by exsolved Ni-Co alloy nanoparticles for high-efficiency CO 2 electrolysis. The cell renders a higher activity for electrolysis of CO 2 with a current density of 1.53 A cm−2 @2.0 V and 850 °C. Faradic efficiency measurement and stability test suggest that LSTNC-r are promising fuel electrodes for high-efficient CO 2 electrolysis. [ABSTRACT FROM AUTHOR]