AbstractAlthough In2O3 nanofibers (NFs) are regarded as one of the active channel materials for next‐generation, low‐cost thin‐film transistors (TFTs), these NFs‐based devices still suffer from the degraded carrier mobility and operational instability, limiting the ability of such devices to replace current polycrystalline silicon technologies. Here, it is shown that nanofiber channel transistors with high electron mobility and operational stability can be achieved by selectively doping Zn element into electrospun In2O3 NFs. By precisely manipulating the doping level during NFs fabrication, their crystallinity, surface morphology, and corresponding device performance can be regulated reliably for enhanced transistor performances. It has been detected that InZnO/SiO2 TFTs with an optimized Zn doping concentration of 50% have demonstrated the high field‐effect mobility (µFE) of 6.38 cm2 V−1 s−1, the larger ION/IOFF of 4.12 × 107 and operation in the energy‐efficient enhancement‐mode. Low frequency noise (LFN) measurements have displayed that the scattering and defects inside the NFs are effectively suppressed by the particular microstructure. When integrating ALD‐derived Al2O3 films as the gate dielectric into TFTs devices, their electron mobility and ION/IOFF can be further improved to 37.82 cm2 V−1 s−1 and 2.92 × 108, respectively. To demonstrate the potential toward more complex logic applications, a low voltage resistor‐loaded unipolar inverter is built by using InZnO/Al2O3 TFT, exhibiting a high gain of 20.95 and full swing characteristics. These optimized parameters have demonstrated the significant advance of this electrospinning technique toward practical applications for high performance and large‐scale electronics.