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Carbon deposition on Ni-based anode is well-known as a major barrier for the practical use and commercialization of hydrocarbon-fuelled solid oxide fuel cells (SOFCs). In this work, Co alloying in Ni-YSZ was studied as an alternative anode material for using CH4 as a fuel. The Ni-YSZ and Ni-Co alloyed-YSZ were prepared by the traditional impregnation method without further mixing processes. After sintering and reduction in H2 atmosphere, the introduced Co can completely dissolved into the Ni lattice and changed the morphology with an increase in the Ni-YSZ grain size and showed a better uniform microstructure. The Co alloying also enhanced the electrochemical performance under CH4 fuel by reducing the resistance and anodic overvoltage. Moreover, the Co addition enhanced the stability of the cell with CH4 a constant load current of 80 mA for 60 h. This performance related to the carbon deposition on the anode surface. The Co alloying showed a high efficiency to suppress the carbon deposition and improved the electrochemical performance of an SOFC cell operating under CH4 fuel.