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BaZr0.8Y0.2O3−δ (BZY) is an excellent candidate material for hydrogen permeation membranes due to its high bulk proton conductivity, mechanical robustness, and chemical stability in H2O- and CO2-containing environments. Unfortunately, the use of BZY as a separation membrane has been greatly restrained by its highly refractory nature, poor grain boundary proton conductivity, high number of grain boundaries resulting from limited grain growth during sintering, as well as low electronic conductivity. These problems can be resolved by the fabrication of a Ni–BZY composite membrane with large BZY grains, which requires the development of a sinteractive Ni–BaZr0.8Y0.2O3−δ materials system. In this work, Ni–BZY composite membranes have been fabricated by three methods: (i) a combined EDTA-citric method, (ii) a solid state reactive sintering method, and (iii) a solid state reaction method. The effects of …