Polymers crosslinked by covalent bonds suffer from a conflict: dense covalent crosslinks increase modulus but decrease fatigue threshold. Polymers crosslinked by physical bonds commonly have large hysteresis. Here we simultaneously achieve high modulus, high fatigue threshold, and low hysteresis in a network of unusually long polymer chains crosslinked by domains of physical bonds. When the network without precrack is pulled by a moderate stress, chains in the domains slip negligibly, so that the domains function like hard particles, leading to high modulus and low hysteresis. When the network with a precrack is stretched, the chains in the domains at the crack tip slip but do not pull out. This enables high tension to transmit over long segments of chains, leading to a high fatigue threshold.

Dielectric elastomers (DEs) are promising electroactive artificial muscles for use in soft machines. However, achieving anisotropy and sub-kV actuation voltage remains a great challenge for DE actuators. Herein, we report a facile method to fabricate ultrathin anisotropic DE films of an amorphous triblock copolymer poly(styrene-b-butyl acrylate-b-styrene) (SBAS) for soft actuators. The modulus of anisotropic SBAS in one direction can be modulated from 0.3 MPa to 10.5 MPa, and the modulus in the orthogonal direction remains the same as that of the pristine film (0.3 MPa). The anisotropy endows soft DE actuators with the directional-preferred response to an applied electric field and programmable multiple actuation morphs. These anisotropic SBAS films allowed us to fabricate compact soft robotics with high maneuverability, including soft grippers for object manipulation and crawling robots with reversible moving ability under an actuation voltage around 800 V.