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Zirconia-toughened alumina (ZTA)/Al₂TiO₅ composites were prepared via a sol–gel route. The prepared samples were uniaxially pressed and pressurelessly sintered at 1650–1700 °C for 1 h. The microstructure, densification, and X-ray diffraction patterns of the sintered ZTA/Al₂TiO₅ composites were investigated, and their mechanical properties, thermal coefficient, and shock resistance were characterized. The addition of Al₂TiO₅ hindered the grain growth of the alumina particles and enhanced the relative density, Vickers hardness, and bending strength of the composites compared with pure ZTA samples. The fracture toughness was improved by 19% upon the addition of 40 wt% Al₂TiO₅. Moreover, increasing the Al₂TiO₅ content resulted in an improvement in the thermal shock resistance.