Work

Porous hierarchically ordered hydrogels demonstrating structurally dependent mechanical properties

Year: 2025

Type: article

Abstract: While hierarchical ordering is a distinctive feature of natural tissues and is directly responsible for their diverse and unique properties, efforts to synthesize biomaterials have primarily focused on using molecular-based approaches with little emphasis on multiscale structure. Here, we report a bottom-up self-assembly process to produce highly porous hydrogel fibers that resemble extracellular matrices both structurally and mechanically. Physically crosslinked nanostructured micelles form the walls of micrometer-sized water-rich pores with preferred orientation along the fiber direction. Low elastic moduli (<1 kPa), high elasticity (extending by more than 12 times the initial length), non-linear elasticity (e.g., hyperelasticity), and completely reversible extension are derived from unevenly distributed strain between the micrometer-sized pores and the polymer chains, which is reminiscent of cellular solids. Control of the material microstructure and orientation over many orders of magnitude (e.g., nm–μm), while holding the nanostructure constant, reveals how the multiscale structure directly impacts mechanical properties. Hierarchical ordering is critical for preparing biomimetic materials, but control of multiscale structure over many length scales is limited. Here, the authors report on a bottom-up assembly process for producing highly porous hydrogel structures where structure dictates bulk properties.

Source: Nature Communications

DOI: 10.1038/s41467-025-59171-w