The possibilities to grow thin films of SrTiO3 and Al2O3 by atomic layer deposition for stacked metal–insulator–metal capacitors have been investigated in this work. In order to tune the functional properties of the capacitors, different processing steps have been employed to realize different combinations of the dielectric stacks. Electrical properties, extracted after the postdeposition annealing and sputter deposition of the Au top electrodes, indicated that the metal–insulator–metal (MIM) structures with additional Al2O3 layer provided better leakage currents densities, compared to the ones with single SrTiO3 based MIM capacitors, but the dielectric constant values have also decreased if additional Al2O3 film was inserted. Attempts to optimize the properties of the MIM stacks have been done by manufacturing heterostructures of Al2O3/SrTiO3/Al2O3 as well as SrTiO3/Al2O3/SrTiO3. In the first case, Al2O3 prevented the crystallization of SrTiO3 in the multilayer dielectric structure and therefore reduced the total capacitance density of the particular MIM stack, whereas the SrTiO3/Al2O3/SrTiO3 stack was found to possess superior electrical properties. Leakage current density as low as ∼10−8 A/cm2 at 2 V and the dielectric constant value of 40 have been extracted.