Nickel oxide yttria-stabilized zirconia (NiO-YSZ) anode materials were synthesized via hydrolysis of the corresponding chloride solutions with NH3, NH3+NaOH, and NaOH as precipitation agents. Powder properties such as crystallite size, morphology, and sintering behavior of the final NiO-YSZ materials were also studied. The mechanism of the formation of NiO-YSZ was established for the different co-precipitation techniques by the direct observation of Ni(NH3)(n)(+2) complexes, Ni(OH)(2) and NiO at different stages of the synthesis process. A direct relationship between the precipitation agent, the order of calcination from dry sample to final product, the final composition, the crystallite sizes and particle sizes of NiO, and the sinterability of the final products was established. A comparison of the powder and individual component properties indicate that the choice of precipitation agent greatly influences the final characteristics. Ni/YSZ materials prepared by NH3+NaOH precipitation offer higher Ni dispersion and nanocrystallinity of both the Ni and YSZ phases. The conductivity of both prepared materials compares well with mixed-oxide materials of higher Ni content.