Photo‐, Thermal‐, and Electro‐Responsive Polyolefin‐Based Actuators

Abstract Stimuli‐responsive polymeric actuators have been applied in soft robotics and artificial muscles. Although numerous functional polymers are used during actuator fabrication, the utilization of low‐cost and industrially scalable polyolefins has remained largely unexplored. This study presents a facile in situ polymerization strategy to fabricate multifunctional polyolefin‐based actuators with exceptional mechanical strength, rapid stimuli‐responsiveness, and ultrahigh work capacities. By developing PANI/CNTs‐COOH composite fillers as catalytic supports for α‐diimine nickel catalysts, in situ ethylene polymerization was used to produce a uniform dispersion of functional fillers within a branched polyethylene matrix. This overcame the phase separation inherent to traditional blending methods. The resulting composites demonstrated remarkable mechanical properties, reaching a maximum tensile stress of 135 MPa after training, a tunable electrical conductivity, and a high photothermal conversion efficiency. These properties enabled self‐healing and triple‐stimuli‐responsive shape‐memory behavior. When used as actuators, these materials exhibited programmable actuation with a work capacity of 470.4 J kg −1 .