Thin-film transistors (TFTs) have drawn widespread applications in the increasingly sophisticated display field. Despite the mature process of fabricating enhancement-mode TFTs, lack of facile methods to realize depletion-mode TFTs restrains the implementation of complementary-type circuits, which in turn leads to relatively high power. Here, the supercritical fluid technique is introduced to elaborately design and tune the interface, providing the opportunity for function-mode transformation of TFTs. By harnessing supercritical-assisted ammoniation (SCA) treatment, interfacial polarization induces negative shift of threshold voltage (from 0.2 to −9.8 V), which allows TFTs to remain normally on-state in the absence of complex capacitor-integrated circuits. This convenient technique, without an additional manufacturing process to achieve function-mode transformation, can thus enable the fabrication of comprehensive-mode TFTs under the same process. Furthermore, comprehensive optimizations in the mobility (increases from 2.08 to 17.12 cm 2 V −1 s −1 ), leakage current (reduces from 1.33 × 10 −11 to 2.22 × 10 −12 A), hysteresis (reduces from 11.2 to 0.2 V), and on/off current ratio (increases from 9.65 × 10 4 to 7.98 × 10 6 ) are achieved simultaneously. Based on conjoint analysis of electrical and material characterization, a reaction model is established for a clearer understanding of the interfacial polarization process. Overall, this lowtemperature SCA treatment offers an environmentally benign strategy to modulate the function mode of electronic devices via interfacial engineering and optimize device performance at the same time, exhibiting promise in promoting the implementation of complementary, low-power circuit.