Ferroelectric‐Gated Hybrid‐Layered Organic Field‐Effect Transistors for Multimode Signal Processing

The rapid development of intelligent systems has driven the urgent need for multifunctional devices within a unified framework through innovative design principles. Here, a ferroelectric‐gated organic field‐effect transistor (Fe‐OFET) is proposed, which synergistically combines light perception, data storage, and neuromorphic computing functionalities. The device features a hybrid‐layered channel with engineered organic molecule modification, improving photodetection performance via optimized exciton dissociation, electron trapping, and hole injection. This design yields exceptional photoresponsivity of 2.4 A W −1 and detectivity of 1.3 × 10 13 Jones. Integration of the ferroelectric layer enables nonvolatile conductance modulation, exhibiting a wide memory window, robust switching endurance with an on/off ratio of >10 4 and long‐term data retention exceeding 4 × 10 3 s. Furthermore, the Fe‐OFET‐based synapse architecture demonstrates potential for wearable neuromorphic electronics, combining flexibility with cognitive functions. The device demonstrates accurate recognition and classification of electrocardiogram waveforms and handwritten digits, achieving accuracies up to 85% and 91%, respectively. This work establishes a hardware paradigm in multimode signal processing and adaptive edge intelligence, offering innovative solutions for next‐generation electronics targeting diverse application scenarios.