Polyisobutylene Encapsulated PEDOT: Pss Electrode Honeycomb Skeleton Electrolyte for Moisture Resistant Electro‐Ionic Soft Artificial Muscles

Abstract Advances in electro‐ionic soft actuators hold significant potential as next‐generation bioelectronic interfaces due to mechanical compliance and operation in agreement with soft biological tissues and low voltages. However, current devices call for encapsulation strategies to accommodate high mechanical demands and long‐term stability in environmental changes. In this study, a durability of polyvinylidene‐fluoride‐co‐hexafluoropropylene (PVDF‐co‐HFP) honeycomb skeleton electrolyte encapsulated with a biocompatible polyisobutylene (PIB) thin film is being investigated. A low water vapor transmission rate (0.61 g m⁻² day⁻¹) and elastic modulus (10 kPa) are measured from a 7.5 µm‐thick thin‐modified PIB‐encapsulation layer. The PIB‐encapsulated soft actuator maintains 68% of its mechanical durability after 40 000 cycles of zero‐to‐tension fatigue loading at room temperature. A cantilever actuation test of the PIB‐encapsulated 3mm‐wide 30mm‐long actuator film shows a large tip displacement (15.90 mm) at a low voltage (±1.5 V) under 0.1 Hz, 37 °C, 50% relative humidity (RH). Most importantly, while the unencapsulated actuator immediately degrades in a few cycles at 37 °C, 50%RH, and 0.1% applied strain, PIB‐encapsulated soft actuator performs up to 6500 dynamic actuation cycles without any functionality degradation. Exceptional durability against mechanical fatigue and stability at elevated temperature and humidity meet the prerequisite for future soft biomedical robots that enable long‐lasting safe operations.