Symmetric three-layer porous alumina/zirconia composites with controlled “designer” pore structure have been prepared by a tertiary-butyl alcohol-based freeze casting and sintering at 1400–1500°C in air. Unidirectional aligned macropore channels were developed over a long range by controlling the solidification direction of tertiary-butyl alcohol solvent; in this case, they were surrounded by more dense structured walls. In layered composite, the bottom layer consisted of small sized pore channels (∼11μm in diameter) compared with the middle and the top layer, due to the comparatively rapid velocity of the TBA crystal growth during solidification. The compressive strength (63–376MPa) of the sintered porous layered composite remarkably increased as the porosity decreased (64–32%).