A new strategy is reported to achieve high‐mobility, low‐off‐current, and operationally stable solution‐processable metal‐oxide thin‐film transistors (TFTs) using a corrugated heterojunction channel structure. The corrugated heterojunction channel, having alternating thin‐indium‐tin‐zinc‐oxide (ITZO)/indium‐gallium‐zinc‐oxide (IGZO) and thick‐ITZO/IGZO film regions, enables the accumulated electron concentration to be tuned in the TFT off‐ and on‐states via charge modulation at the vertical regions of the heterojunction. The ITZO/IGZO TFTs with optimized corrugated structure exhibit a maximum field‐effect mobility >50 cm2 V−1 s−1 with an on/off current ratio of >108 and good operational stability (threshold voltage shift <1 V for a positive‐gate‐bias stress of 10 ks, without passivation). To exploit the underlying conduction mechanism of the corrugated heterojunction TFTs, a physical model is implemented by using a variety of chemical, structural, and electrical characterization tools and Technology Computer‐Aided Design simulations. The physical model reveals that efficient charge manipulation is possible via the corrugated structure, by inducing an extremely high carrier concentration at the nanoscale vertical channel regions, enabling low off‐currents and high on‐currents depending on the applied gate bias. High‐performance and controllable metal oxide semiconductors utilizing a corrugated bilayer structure are achieved, which display enhanced mobility and control of carrier concentration, corresponding to the operation states of the device. This novel strategy can be used as a general route to high‐mobility, extremely stable, and controllable semiconductor devices, offering compatibility with standard complementary metal‐oxide‐semiconductor (CMOS) processing and large‐scale on‐chip device applications.