In this work, bi-layered Fe–Ni–Co–YSZ/YSZ nanostructured composites for solid oxide fuel cells were obtained using the spark plasma sintering (SPS) technique. The microstructures of the anode and electrolyte were controlled by optimization of SPS consolidation parameters. The resulting bilayers have a full dense YSZ electrolyte and porous Fe–Ni–Co/YSZ anode as well as crack-free and well-bonded anode/electrolyte interface. On the other hand, SPS under non-optimized processing parameters cannot yield the desired results. The high resistance to thermal stresses of the fabricated half-cells was achieved with Fe–Ni–Co/YSZ anode. The developed anode showed higher thermal compatibility with YSZ electrolyte than usual Ni/YSZ cermet. Thus, with the successful combination of SPS parameters and anode material, we have obtained bi-layers for SOFCs with required microstructure and thermal compatibility.