NaCl-type (B1) chromium oxide (CrO) has been expected to have a high hardness value and does not exist as an equilibrium phase. We report a B1-based Cr0.67O thin film with a thickness of 144 nm prepared by pulsed laser deposition as an epitaxial thin film on a MgO single crystal. The thin film contained a number of stacking faults and had a nanotwinned structure composed of B1 with disordered vacancies and corundum structures. The Cr0.67O thin film had a high indentation hardness value of 44 GPa, making it the hardest oxide thin film reported to date.
