Biomimetic assembly of organic ferroelectrics induced tailorable domain reconfiguration for high-performance self-powered neuromorphic system

The pursuit of self-powered neuromorphic systems confronts a fundamental trade-off: reconciling synaptic functionality, energy autonomy, and mechanical compliance with sustainable fabrication. Herein, we break this dilemma through a biomimetic four-leaf microstructure with size-tunability, constructed via single-step self-assembly of molecular ferroelectrics ( R )-3-Quinuclidinol (R-3-Q) and ferroelectric polymer poly(vinylidene fluoride- co -trifluoroethylene) (P(VDF-TrFE)). These microstructures induce domain reconfiguration and realize ideal synaptic plasticity, including impressive paired pulse facilitation (PPF) / paired pulse depression (PPD) indices (284.7/290.5), satisfactory linearity (α LTP /α LTD  = 0.08624/0.09185), and excellent symmetry (ANL = 0.00367). Moreover, they enable stress-locked piezoelectric amplification and achieve considerable electrical output ( V oc  = 24.0 V). The synergy of these effects creates a highly-efficient and self-powered neuromorphic system that directly encodes multidimensional mechanical inputs into feature-specific synaptic responses, demonstrating real-time tactile adaption. By harmonizing bioinspired domain engineering with scalable self-assembly strategy, this work pioneered a universal paradigm in human-machine interaction, adaptive neuroprosthetics/robotic skins, metaverse interfaces and embodied intelligence systems.