Messy or Ordered? Multiscale Mechanics Dictates Shape‐Morphing of 2D Networks Hierarchically Assembled of Responsive Microfibers

Shape‐morphing active networks of mesoscale filaments are a common hierarchical feature in biology for applying forces, transporting materials, and inducing motility with microscale resolution. Synthetic morphing systems of similar dimensions and capabilities hold potential for a range of technological applications, from micro‐muscles to shape‐morphing optical devices. Here, the fabrication of highly‐ordered 2D networks hierarchically constructed of thermoresponsive mesoscale polymeric fibers, which can exhibit morphing with microscale resolution, is presented. It is demonstrated both experimentally and computationally that the morphing of such networks strongly depends on the physical attributes of the single fiber, in particular on two intrinsic length scales—the fiber diameter and mesh size, which stems from network's density. It is shown that depending on these parameters, such fiber‐networks exhibit one of two thermally driven morphing behaviors: i) the fibers stay straight, and the network preserves its ordered morphology, exhibiting a bulk‐like behavior; or ii) the fibers buckle and the network becomes messy and highly disordered. Notably, in both cases, the networks display memory and regain their original ordered morphology upon shrinking. This hierarchically induced phase transition, demonstrated here on a range of networks, offers a new way of controlling the shape‐morphing of synthetic materials with mesoscale resolutions. Shape‐morphing Cartesian 2D networks of microscale thermoresponsive fibers are fabricated using the jet‐writing approach. The networks exhibit two morphing behaviors: i) shape‐preserving, which keeps the Cartesian morphology, or ii) disordered swelling into a messy network. The factors controlling this transition are analyzed and modeled, providing a novel strategy for designing functional materials with microscale morphing resolutions and unique morphing abilities.