The manipulation of antiferromagnetic order in magnetoelectric Cr2O3 using electric field has been of great interest due to its potential in low-power electronics. The substantial leakage and low dielectric breakdown observed in twinned Cr2O3 thin films, however, hinders its development in energy efficient spintronics. To compensate, large film thicknesses (250 nm or greater) have been employed at the expense of device scalability. Recently, epitaxial V2O3 thin film electrodes have been used to eliminate twin boundaries and significantly reduce the leakage of 300 nm thick single crystal films. Here we report the electrical endurance and magnetic properties of thin (less than 100 nm) single crystal Cr2O3 films on epitaxial V2O3 buffered Al2O3 (0001) single crystal substrates. The growth of Cr2O3 on isostructural V2O3 thin film electrodes helps eliminate the existence of twin domains in Cr2O3 films, therefore significantly reducing leakage current and increasing dielectric breakdown. 60 nm thick Cr2O3 films show bulk-like resistivity (~ 1012 Ω cm) with a breakdown voltage in the range of 150–300 MV/m. Exchange bias measurements of 30 nm thick Cr2O3 display a blocking temperature of ~ 285 K while room temperature optical second harmonic generation measurements possess the symmetry consistent with bulk magnetic order.