Coatings with tunable refractive index and high mechanical resilience are useful in optical systems. In this work, thin films of HfO2doped with Al2O3were deposited on silicon at 300 °C by using plasma-enhanced atomic layer deposition (PE-ALD). The mainly amorphous 60–80 nm thick films consisted Al in the range of 2 to 26 at.%. The refractive indexes varied from 1.69 to 2.08 at the wavelength of 632 nm, and they consistently depended on the composition. The differences were higher in the UV spectral region. At the same time, the hardness of the films was from 12–15 GPa; the modulus was in the range of 160–180 GPa; and the mechanical properties did not have a good correlation with the deposited compositions. The deposition conditions, element contents, and refractive indexes at respective wavelengths were correlated. The results indicated that it is possible to tune optical properties and retain mechanical properties of atomic layer-deposited thin films of HfO2with Al2O3as doping oxide. Such films could be used as mechanically resilient and optically tunable coatings in, for instance, micro- or nano-electromechanical systems or transparent displays.