Physical Anchoring‐Assisted Mechanically Guided Assembly for Material‐Independent 3D Mesostructures

ABSTRACT Mechanically guided 3D assembly has emerged as a powerful approach for constructing complex mesostructures, but conventional strategies rely on selective chemical bonding between 2D precursors and elastomeric substrates, restricting material compatibility and scalability. Here, we introduce a physical anchoring‐based, buckling‐guided assembly platform that decouples 3D structure formation from chemical adhesion. The platform employs an elastomeric substrate patterned with an array of rods to achieve robust mechanical fixation, enabling the integration of diverse functional materials, including polymers, metals, water‐soluble polymers, and stimuli‐responsive systems, independent of their interfacial or mechanical properties. Oxygen plasma surface treatment further reduces adhesion, allowing reliable assembly of freestanding and large‐area architectures. As a proof‐of‐concept, we integrate liquid crystalline networks (LCNs) to demonstrate light‐responsive soft robotic systems capable of remote actuation. This physically anchored assembly strategy establishes a general and scalable framework for mesoscale fabrication, expanding material and geometric design freedom for applications in soft robotics, bioelectronics, and multi‐material integration.