We demonstrate a low-temperature layer-by-layer formation of a metal-oxide-only (AlOx) gate dielectric to attain low-voltage operation of a self-assembly based vertical organic field effect transistor (VOFET). The AlOx deposition method results in uniform films characterized by high quality dielectric properties. Pin-hole free ultrathin layers with thicknesses ranging between 1.2 and 24 nm feature bulk dielectric permittivity, εAlOx, of 8.2, high breakdownfield (>8 MV cm(-1)), low leakage currents (<10(-7) A cm(-2) at 3MV cm(-1)), and high capacitance (up to 1 μF cm(-2)). We show the benefits of the tunable surface properties of the oxide-only dielectric utilized here, in facilitating the subsequent nanostructuring steps required to realize the VOFET patterned source electrode. Optimal wetting properties enable the directional block-copolymer based self-assembly patterning, as well as the formation of robust and continuous ultrathin metallic films. Supported by computer modeling, the vertical architecture and the methods demonstrated here offer a simple, low-cost, and free of expensive lithography route for the realization of low-voltage (VGS/DS≤3 V), low-power, and potentially high-frequency large-area electronics.

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