Liquid Crystal Elastomers Micro-Supercapacitors with Robust Interfacial Integration for Untethered Soft Robotics

Untethered integrated energy-actuation systems are desirable for soft robots to break their long-standing dependence on external power tethers. However, it remains challenging to develop stable functional modules with robust interfacial integrity that endure repetitive actuation without delamination. Herein, we report thermally driven micro-supercapacitor (TD-MSC) soft modules fabricated via direct ink writing of MXene/ TEMPO-oxidized bacterial cellulose (TOBC) electrodes on plasma-activated liquid crystal elastomers (LCEs). A strong dual-coupled interface with synergistic non-covalent and covalent bonding is constructed via a trimethylolpropane tris(3-mercaptopropionate) (TMPTMP) and trimethylolpropane triacrylate (TMPTA) click chemistry-based electrolyte. The resulting TD-MSCs deliver an areal capacitance of 106.12 mF cm^{- 2} and retain 69% capacitance after 5000 cycles, benefiting from TOBC-enabled ion transport pathways and enhanced mechanical integrity. The device achieves controllable, reversible thermally-driven deformation, enabling biomimetic peristalsis motion while maintaining robust interfacial bonding and stable electrochemical performance. Importantly, distinct actuation modules can be realized by tailoring the spatial arrangement of the electrodes. As a proof-of-concept illustration, untethered integrated soft systems with onboard energy storage capable of heavy-duty grasping and state sensing are constructed by integrating TD-MSCs with thermally responsive control circuits. This work demonstrates an integrated energy-actuation architecture and provides a promising strategy for multifunctional soft robotic systems with environmental interaction.