Magnetically Driven Hierarchical Alignment in Biomimetic Fibrous Hydrogels

In vivo, natural biomaterials are frequently anisotropic, exhibiting directional microstructures and mechanical properties. It remains challenging to develop such anisotropy in synthetic materials. Here, a facile one-step approach for in situ fabrication of hydrogels with hierarchically anisotropic architectures and direction-dependent mechanical properties is proposed. The anisotropic hydrogels, composed of a fibrous gel network (0.1 wt%), cross-linked with magnetic nanoparticles (spheres, rods, and wires, <0.1 wt%) are readily formed in the presence of very low magnetic fields (<20 mT). The anisotropy of the nanoparticles is transduced to the polymer network, leading to macroscopic anisotropy, for instance, in mechanical properties. Electrostatic repulsion by the negatively charged nanoparticles induces an additional layer of order in the material, perpendicular to the magnetic field direction. The straightforward fabrication strategy allows for stepwise deposition of layers with different degrees or directions of anisotropy, which enables the formation of complex structures that are able to mimic some of the complex hierarchical architectures found in biology. It is anticipated that this approach of hydrogel alignment may serve as a guide for designing advanced biomaterials in tissue engineering.