Abstract The atomic layer deposition (ALD) of HfO2 and ZrO2 thin films is investigated using (MeCp)2HfMe2, (MeCp)2Hf(OMe)(Me), (MeCp)2ZrMe2, and (MeCp)2Zr(OMe)(Me) as the precursors at deposition temperatures between 300 and 500 °C, with water vapor as the oxygen source. A self‐limiting growth mechanism is confirmed at 350 °C for all the metal precursors examined. The processes provide nearly stoichiometric HfO2 and ZrO2 films with carbon and hydrogen concentrations below 0.5 and 1.0 at.‐%, respectively, for representative samples. All films are polycrystalline as deposited, and possess a thin interfacial SiO2 layer. The capacitance‐voltage (C‐V) and current density‐voltage (I‐V) behavior is reported and discussed for capacitor structures containing films from this study.