Abstract: Magnetoactive soft materials, typically composed of magnetic particles dispersed in a soft polymer matrix, are finding many applications in soft robotics due to their reversible and remote shape transformations under magnetic fields. To achieve complex shape transformations, anisotropic, and heterogeneous magnetization profiles must be programmed in the material. However, once programmed and assembled, magnetic soft actuators cannot be easily reconfigured, repurposed, or repaired, which limits their application, their durability, and versatility in their design. Here, magnetoactive soft composites are developed from squid-derived biopolymers and NdFeB microparticles with tunable ferromagnetic and thermomechanical properties. By leveraging reversible crosslinking nanostructures in the biopolymer matrix, a healing-assisted assembly process is developed that allows for on-demand reconfiguration and magnetic reprogramming of magnetoactive composites. This concept in multi-material modular actuators is demonstrated with programmable deformation modes, self-healing properties to recover their function after mechanical damage, and shape-memory behavior to lock in their preferred configuration and un-actuated catch states. These dynamic magnetic soft composites can enable the modular design and assembly of new types of magnetic actuators, not only eliminating device vulnerabilities through healing and repair but also by providing adaptive mechanisms to reconfigure their function on demand.

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