Composite tetragonal zirconia (3Y-TZP) sinters with Al2O3 contents of 0, 1, 5, 10 and 15 mol% were obtained from a 3-YSZ powder prepared using the gelatin method, and the influence of alumina addition on the mechanical and electrical properties of the obtained sinters was investigated. Al2O3 was added via two different methods, namely during the preparation of the 3-YSZ powder and via impregnation using an alcohol solution of aluminum nitrate. The obtained green bodies were sintered for 2 h in air at 1773 K. The structure and morphology of the two series of sinters were investigated using XRD and SEM-EDS, their electrical properties were determined using impedance spectroscopy, and their hardness and critical stress intensity factor were measured using the Vickers indentation test. We established that both the amount of alumina and the method used to introduce it into the 3Y-TZP matrix significantly affect the physicochemical properties of the obtained polycrystalline material. The 3-YSZ/10 mol% Al2O3 sinter that had Al2O3 introduced during the preparation of the 3-YSZ powder was found to exhibit the most advantageous mechanical and electrical properties while still having sufficiently low porosity.