The memory structures Pt/Al2O3/(TiO2)x(Al2O3)1−x/Al2O3/p-Si(nominal composition x = 0.05, 0.50 and 0.70) were fabricated by using rf-magnetron sputtering and atomic layer deposition techniques, in which the dielectric constant and the bottom of the conduction band of the high-k composite (TiO2)x(Al2O3)1−x were adjusted by controlling the partial composition of Al2O3. With the largest dielectric constant and the lowest deviation from the bottom of the conduction band of Si, (TiO2)0.7(Al2O3)0.3 memory devices show the largest memory window of 7.54 V, the fast programming/erasing speed and excellent endurance and retention characteristics, which were ascribed to the special structural design, proper combination of dielectric constant and band alignment in the high-k composite (TiO2)0.7(Al2O3)0.3.