A highly active anode material for solid oxide fuel cells resistant to carbon deposition is developed. Co-Fe co-doped La 0.5 Ba 0.5 MnO 3- with a cubic-hexagonal heterogeneous stucture is synthesized through the Pechini method. An A-site ordered double perovskite with Co 0.94 Fe 0.06 alloy-oxide core-shell nanoparticles on its surface is formed after reduction. The phase transition and the exsolution of the nanoparticles are investigated with X-ray diffraction, thermogravimetric analysis, and high-resolution transmission electron microscope. The exsolved nanoparticles with the layered double-perovskite supporter show a high catalytic activity. A single cell with that anode and a 300 μm thick La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3 electrolyte layer exhibits maximum power densities of 1479 and 503 mW cm -2 at 850 °C with wet hydrogen and wet methane fuels, respectively. Moreover, the single cell fed with wet methane exhibits a stable power output at 850 °C for 200 h, demonstrating a high resistance to carbon deposition of the anode due to the strong anchor of the exsolved nanoparticles on the perovskite parent. The oxide shell also preserves the metal particles from coking.