Atomic layer deposition of hafnium−titanium-oxide (Hf x Ti 1−x O y ) films on silicon substrates and Ru, RuO 2 , and Pt seed layers was investigated. The films were grown using HfCl 4 and TiCl 4 as the metal precursors and H 2 O and O 3 as the oxygen precursors. At a temperature of 350 °C and x ≤ 0.12, tetragonal phases isomorphous with anatase-and rutile-phase TiO 2 grew on silicon and on Ru and RuO 2 , respectively. The films with 0.3 ≤ x ≤ 0.65 grown on silicon and Pt were amorphous, while those deposited on Ru and RuO 2 contained the crystal structure isomorphous with orthorhombic HfTiO 4 . Independently of substrates, the phase isomorphous with monoclinic HfO 2 was formed in the films with 0.73 ≤ x ≤ 1.0. The crystal structure influenced the concentration of chlorine impurities that was lower in crystalline films grown on Ru and RuO 2 at 350−400 °C than that in amorphous films simultaneously deposited on Si. No significant effect of substrates on the chlorine concentrations was revealed for amorphous films deposited on Si, Ru, and RuO 2 at 250 °C. The relative permittivity measured at 10 kHz for Hf x Ti 1−x O y grown on RuO 2 ranged from 21 to 90 and monotonically increased with decreasing Hf content.