Printable and flexible electronics attract sustained attention for their low cost, easy scale up, and potential application in wearable and implantable sensors. However, they are susceptible to scratching, rupture, or other damage from bending or stretching due to their “soft” nature compared to their rigid counterparts (Si-based electronics), leading to loss of functionality. Self-healing capability is highly desirable for these “soft” electronic devices. Here, a versatile self-healing polymer blend dielectric is developed with no added salts and it is integrated into organic field transistors (OFETs) as a gate insulator material. This polymer blend exhibits an unusually high thin film capacitance (1400 nF cm −2 at 120 nm thickness and 20–100 Hz). Furthermore, it shows pronounced electrical and mechanical self-healing behavior, can serve as the gate dielectric for organic semiconductors, and can even induce healing of the conductivity of a layer coated above it together with the process of healing itself. Based on these attractive properties, we developed a self-healable, low-voltage operable, printed, and flexible OFET for the first time, showing promise for vapor sensing as well as conventional OFET applications.

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Flexible electronics with highly thermal stability and mechanical strength are highly needed in advanced transportation systems. Semiconducting single‐walled carbon nanotubes are one of the leading active materials for such thin film transistors because they are printable, flexible, thermally stable, and mechanically strong. Dielectrics with large capacitance are another major component, and polymer electrolytes are printed for flexible electronics, but they suffer from poor mechanical strength and low operating temperature. Here, a transparent, mechanically flexible, and thermally stable polyfluorinated electrolyte (PFE) is developed with high capacitance by curing printed polyfluorinated resin (PFR) and ionic liquid composite at high temperature. PFE inherits the mechanical flexibility and thermal stability from PFR. The immobilized ionic liquid inside the porous structures of PFE accounts for the high capacitance. With top‐gated PFE, fully printed electronically pure single‐chirality (6,5) single‐walled carbon nanotube (SWCNT) thin‐film transistors (TFTs) exhibit air stable, consistent, and reliable ambipolar characteristics with high transconductance (1 mS) and small subthreshold swing (<0.15 V dec−1) at low voltage in ambient air for p‐type and n‐type carriers, and >105 ON/OFF current ratio for both carriers under low operation voltage.

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