“…In the current era of the Internet of Things (IoT), flexible electronics has been considered to be one of the most emerging research areas which has garnered significant recognition because of its promising applications in circuits, sensors, radio frequency identification (RFID) tags, rollable displays, human health monitoring, e-textiles, and wearable devices, as well as implantable electronics. − An organic field-effect transistor (OFET) is an essential building block of flexible electronics that has gained tremendous popularity due to its inherent advantages of solution processability, low-temperature processing, ease of integration, low-cost fabrication, and compatibility with rigid as well as flexible substrates such as cloth, paper, plastic skin, etc. ,− The performance of OFETs is determined by various factors starting from the properties of the substrate to the organic semiconductor material, the dielectric, the device structure, and the semiconductor:dielectric interface. ,− A high-quality dielectric:semiconductor interface is preferred to reduce the charge trapping, which is influenced by various factors such as structural defects in the semiconductor film or grain boundaries, surface roughness, polar functional groups, and dielectric constant ( k ) of the gate dielectric. ,− Significant efforts have been made to improve the interfacial properties of the semiconductor:dielectric by introducing hydrophobic self-assembled monolayers (SAMs) or ultrathin polymer films; , however, these inorganic dielectric/SAM combinations lack device flexibility overall. Polymer gate insulators have been considered to be promising candidates for solution-processed flexible OFETs due to their suitability for flexible and large-area processability and the formation of a high-quality dielectric:semiconductor interface. ,, In general, most of these polymer dielectrics have a low dielectric constant (2–5), which poses a critical challenge in obtaining a low operating voltage . Combining these polymer layers with thin high- k metal oxide dielectrics helps in achieving highly oriented semiconductor layers on top of the dielectric and can efficiently protect the channel from external trap-forming moieties .…”