A high-mobility low-voltage graphene field-effect transistor (FET) array was fabricated on a flexible plastic substrate using high-capacitance natural aluminum oxide as a gate dielectric in a self-aligned device configuration. The high capacitance of the native aluminum oxide and the self-alignment, which minimizes access resistance, yield a high current on/off ratio and an operation voltage below 3 V, along with high electron and hole mobility of 230 and 300 cm(2)/V·s, respectively. Moreover, the native aluminum oxide is resistant to mechanical bending and exhibits self-healing upon electrical breakdown. These results indicate that self-aligned graphene FETs can provide remarkably improved device performance and stability for a range of applications in flexible electronics.