Micelle‐Guided Ion Pathways and Graded Polymer Cross‐Linking for Reliable Filament Growth in Organic Memristors

Electrochemical metallization (ECM)‐based organic memristors typically rely on an electroforming step to initiate conductive filament (CF) growth; however, this process is often prolonged and unreliable due to uncontrolled ion migration. Despite considerable efforts, achieving stable and reliable organic ECM devices through a simple, solution‐process‐compatible method remains challenging. Here, we introduce a bilayer organic memristor architecture that confines ion‐migration pathways, in which a micelle‐engineered transport layer (PT) is integrated with a crosslinked confinement layer (PG). A bilayer organic memristor integrates micelle‐engineered PT and crosslinked PG layers to guide vertical Ag + ion migration and confine filament growth, suppressing the electroforming requirement. The resulting device exhibits low‐voltage operation (∼0.5 V), a high on/off ratio (∼10 5 ), and stable data retention exceeding 3600 s. Moreover, crossbar array implementation demonstrates strong potential for neuromorphic computing and large‐scale integration, where reproducibility and energy efficiency are critical. Owing to their solution‐processable and polymer‐based nature, these devices are also well suited for low‐cost, flexible, and wearable electronic systems.