Nanocrystalline nickel oxide–yttrium-stabilized zirconia (NiO/YSZ) composite powder for the solid oxide fuel cells was prepared by solution combustion through control of pH values and contents of glycine fuel in precursor solution. A strongly acidic precursor solution with appropriate amounts of glycine fuel added increased the specific surface area of the synthesized composite powders. This results from the increased binding of metal ions and glycine under strongly acidic solution (pH = 0.5) conditions. After sintering and reducing treatment of nanocrystalline NiO/YSZ composite, the Ni/YSZ pellet showed an ideal microstructure: fine Ni particles of 3 to 5 μm were distributed uniformly, and fine micropores around Ni metal particles were formed, thus leading to an increase in the triple phase boundary area among gas, Ni and YSZ.