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In this study, an asymmetric NiO–yttria-stabilized zirconia (YSZ) cathode substrate has been successfully fabricated by the phase-inversion tape casting method. 3-dimensional X-ray microscopy and subsequent analysis demonstrate that the NiO–YSZ substrates exhibit dual-layer structure: a thin sponge-like pore layer is supported on a thick finger-like macro-void layer. The electrochemical performance of the Ni–YSZ/YSZ/YSZ–LSM electrolyzer with this novel dual-layer cathode has been significantly enhanced. The electrolyzer exhibits an excellent current density of 2.3 A cm^− 2 and a high H₂ production rate of 958 mL cm^− 2 h^− 1 at 800 °C and 1.5 V, and a polarization resistance of 0.25 Ωcm² at the open circuit voltage when the cathode and anode are exposed to 33 vol.% H₂O–67 vol.% H₂ and ambient air, respectively, demonstrating that the thin sponge-like pore layer in the dual-layer cathode can provide …