Dual‐Programmable Architected Magnetic Soft Materials: Tuning Mechano–Electric Responses by Inverse Design

ABSTRACT Materials that can deform, sense, and autonomously generate power in response to wireless magnetic fields, through both magnetic‐actuated shape transformation and charge generation, are an emerging focus in advanced functional materials research. Magneto–mechano–electric intelligent materials, created by embedding ferromagnetic particles into soft elastomers with immobile charges, are bringing this vision closer to reality. Under wireless magnetic actuation, they undergo rapid deformation that drives charge flow, enabling controlled responses. Yet realizing such materials to unleash their full potential remains a major challenge because of the complex multiphysics coupling under large deformation and independent mechanical and electrical responses. In this work, we create a new class of dual‐programmable magnetic soft materials with unprecedented dual properties by establishing a multiphysics inverse‐design framework that simultaneously optimizes geometry and remanent magnetization distributions to tune both magneto–elastic and magneto–electric behaviors. The framework is complemented by a tailored fabrication approach and experimental validation, forming a comprehensive and automated pipeline for creating multifunctional advanced materials for biomedical devices with dually programmable behaviors. Its effectiveness is demonstrated through an electrical stimulation guidewire for endovascular therapy, mechano–electric treatment robots for injury‐specific tissue recovery, and multifunctional self‐powering and self‐sensing bio‐robots with on‐demand mechanical motions. Together, these results establish an effective inverse‐design‐to‐fabrication paradigm for dual‐programmable magnetic soft materials in next‐generation biomedical applications.