Atomic layer deposition (ALD) is a useful tool for producing ultrathin films and coatings of complex composition with high thickness control for a wide range of applications. In this study, the growth of zinc–titanium oxide nanofilms was investigated. Diethyl zinc, titanium tetrachloride, and water were used as precursors. The supercycle approach was used, and wide ZnO/TiO2 (ZTO) ALD cycles were prepared: 5/1, 3/1, 2/1, 1/1, 1/2, 1/3, 1/5, 1/10, 1/20. Spectral ellipsometry, X-ray reflectometry, X-ray diffraction, scanning electron microscopy, SEM-EDX, and contact angle measurements were used to characterize the thickness, morphology, and composition of the films. The results show that the thicknesses of the coatings differ considerably from those calculated using the rule of mixtures. At high ZnO/TiO2 ratios, the thickness is much lower than expected and with increasing titanium oxide content the thickness increases significantly. The surface of the ZTO samples contains a significant amount of chlorine in the form of zinc chloride and an excessive amount of titanium. The evaluation of the antibacterial properties showed significant activity of the ZTO–1/1 sample against antibiotic-resistant strains and no negative effect on the morphology and adhesion of human mesenchymal stem cells. These results suggest that by tuning the surface composition of ALD-derived ZTO samples, it may be possible to obtain a multi-functional material for use in medical applications.