A method for the formation of a low-temperature hybrid gate dielectric for high-performance, top-gate ZnO nanowire transistors is reported. The hybrid gate dielectric consists of a self-assembled monolayer (SAM) and an aluminum oxide layer. The thin aluminum oxide layer forms naturally and spontaneously when the aluminum gate electrode is deposited by thermal evaporation onto the SAM-covered ZnO nanowire, and its formation is facilitated by the poor surface wetting of the aluminum on the hydrophobic SAM. The hybrid gate dielectric shows excellent electrical insulation and can sustain voltages up to 6 V. ZnO nanowire transistors utilizing the hybrid gate dielectric feature a large transconductance of 50 μS and large on-state currents of up to 200 μA at gate-source voltages of 3 V. The large on-state current is sufficient to drive organic light-emitting diodes with an active area of 6.7 mm(2) to a brightness of 445 cd/m(2). Inverters based on ZnO nanowire transistors and thin-film carbon load resistors operate with frequencies up to 30 MHz.