Nanocrystalline (nc) ceramic–metal composite bulk samples have been fabricated by consolidation of mixture of attrition-milled (AM) amorphous base ceramic ((ZrO2–3 mol% Y2O3)–20 mol% Al2O3) and AM amorphous base metallic (Ti–48 mol% Al) powders using a pulse-current pressure sintering system. Microstructural observations revealed that the ceramic and metallic colonies appear blocky in morphology in the composite bulk samples, and both the ceramic and the metallic colonies consist of a large number of equiaxed fine grains with the sizes of 78–82 and 81–86 nm, respectively. Mechanical mixing treatments by wet ball milling in ethanol before consolidation process are effective for refinement of the ceramic and metallic colonies. In all the obtained composite bulk samples, the ceramic colonies consist of the dominant phase of tetragonal (t) ZrO2 solid solution (ss) together with the minor phases of monoclinic (m) ZrO2ss and α-Al2O3. On the other hand, the dominant phase in the metallic colonies changes from Ti3Al (α2) to Tiss (α) with an increase in the t-ZrO2ss volume fraction by abrasion of 3 mol% yttria-stabilized tetragonal polycrystalline zirconia balls during wet mechanical mixing treatments. Such a phase transformation from α2 to α is considered to be due to the decrease in the aluminum content in the metallic colonies by combination of aluminum with oxygen (i.e., the formation of α-Al2O3), which is probably taken from ethanol (C2H5OH) into the powders during wet mechanical mixing treatments. The obtained nc composite bulk samples show good Vickers hardness values, which are considerably higher than those estimated from the rule of mixture.