“…The surface, bulk, and interface properties of thin films can be modulated by adjusting the interactions across the macroscopic and atomic scales using molecular-level engineering. − These thin-film properties play notable roles in organic electronics to meet the requirements of next-generation electronics such as printed logic circuits, flexible transistor arrays, and stretchable light-emitting diodes. A gate dielectric layer, which is among the most critical components affecting device performance, and its feasibility in organic field-effect transistors (OFETs) are assessed for (i) good compatibility with organic channel materials and flexible substrates, (ii) compatibility with conventional large-area film deposition methods, (iii) excellent capacitive and insulating properties, (iv) colorless and transparent optical properties, and (v) excellent stability during postdeposition processes. ,− Moreover, controlling the molecular interaction at the interfaces with active layers, which is dominant when the device is in operation, is essential. − For example, gate dielectric materials with polar surface characteristics, which is typical for high dielectric constant materials, may lead to increased charge-trapping sites at their interface with the active layer and band broadening of organic semiconductor (OSC) molecules. − …”