jats:titleAbstract</jats:title> jats:pThe proliferation of place-and-forget devices driven by the exponentially-growing Internet of Things industry has created a demand for low-voltage thin-film transistor (TFT) electronics based on solution-processible semiconductors. Amongst solution-processible technologies, TFTs based on semiconducting single-walled carbon nanotubes (sc-SWCNTs) are a promising candidate owing to their comparatively high current driving capability in their above-threshold region at low voltages, which is desirable for applications with constraints on supply voltage and switching speed. Low-voltage above-threshold operation in sc-SWCNTs is customarily achieved by using high-capacitance-density gate dielectrics such as metal-oxides fabricated via atomic layer deposition (ALD) and ion-gels. These are unattractive, as ALD requires complex-processing or exotic precursors, while ion-gels lead to slower devices with poor stability. This work demonstrates the fabrication of low-voltage above-threshold sc-SWCNTs TFTs based on a high-capacitance-density hybrid nanodielectric, which is composed of a readily-made AlOjats:italic jats:subx</jats:sub> </jats:italic> nanolayer and a solution-processed self-assembled monolayer (SAM). The resultant TFTs can withstand a gate-channel voltage of 1–2 V, which ensures their above-threshold operation with balanced ambipolar behavior and electron/hole mobilities of 7 cmjats:sup2</jats:sup> Vjats:sup−1</jats:sup> sjats:sup−1</jats:sup>. Key to achieving balanced ambipolarity is the mitigation of environmental factors via the encapsulation of the devices with an optimized spin-on polymer coating, which preserves the inherent properties of the sc-SWCNTs. Such balanced ambipolarity enables the direct implementation of CMOS-like circuit configurations without the use of additional dopants, semiconductors or source/drain electrode metals. The resultant CMOS-like inverters operate in the above-threshold region with supply voltages in the 1–2 V range, and have positive noise margins, gain values surpassing 80 V/V, and a bandwidth exceeding 100 kHz. This reinforces SAM-based nanodielectrics as an attractive route to easy-to-fabricate sc-SWCNT TFTs that can operate in the above-threshold region and that can meet the demand for low-voltage TFT electronics requiring moderate speeds and higher driving currents for wearables and sensing applications.</jats:p>