Summary: Zirconium oxide films were prepared using a zirconium arc discharge in a gas mixture of argon‐diluted with oxygen, where the gas flow rate was varied from 100 sccm to 600 sccm, which corresponded to a gas pressure of 1.9 to 4.6 Pa. The voltage applied to the target was, unless otherwise specified, set to a value of −5 kV, with a pulse width of 20 µs at a repetition rate of 400 Hz. It was observed from XPS measurements that the oxygen and zirconium were mostly present in the deposited film in a stoichiometric state. The prepared films changed from amorphous state to orthorhombic structure by increasing the pressure of the gas mixture. At an applied voltage as high as −9 kV, the crystal size becomes small due to high energy ion bombardment. Thus, the structure of the prepared film is changed into a micro‐structural state. By applying a pulse voltage of −5 kV to the substrate, the deposited film shows a smooth surface, with roughness which is smaller by a factor of 1/7 compared to that in the absence of the applied voltage.