In Situ One‐Step Fabrication of Interpenetrating Structures in Liquid Crystal Elastomer Fibers via a Novel Mechanism Coupling Confined Evaporation and Dynamic Chemistry

Liquid crystal elastomers (LCEs) face three critical fabrication challenges: first, the fabrication of complex structures relies on external devices, prone to spatial interference that restricts the design space of topological structures; second, the orientation of liquid crystal (LC) mesogens is dependent on external fields, with precision limited by existing instrumentation; third, the asynchrony between structure formation and orientation induction restricts complex structure fabrication. Herein, we propose an in situ one-step fabrication strategy and successfully fabricate interpenetrating structures that are difficult to realize via conventional approaches. This strategy is based on a novel mechanism, confined evaporation and dynamic chemistry induce ordered topological network formation, which not only broadens the design freedom of complex structures but also achieves three core breakthroughs: autonomous structure regulation via pre-customized confined templates, spontaneous LC mesogens orientation driven by internal stress from confined evaporation, and spatiotemporal synchronization of structure formation and orientation induction enabled by the introduction of dynamic covalent chemistry. Furthermore, we develop an acoustically controllable LCE actuator capable of reversible actuation in response to voice command, realizing acoustically responsive actuation in LCE. This work establishes a novel LCEs fabrication paradigm and reveals the potential of LCEs in acoustic-driven intelligent systems.