LAUSR

The internal modification of natural hierarchical materials can largely improve their inherent properties and afford them new functions. However, conventional methods using small-molecule agents often encounter poor uniformity and low efficiency. By comparing the penetration of small molecules and nanoparticles into hierarchical collagen fibers, we propose a general strategy, namely modular penetration and controlled release (MP-CR), for the internal modification of 3D biomass materials. We demonstrate that nano-sized aluminum-loaded particles can penetrate into collagen networks more effectively and evenly than small-molecule crosslinkers. After the on-demand pH-triggered release of interactive aluminum ions, enhanced internal crosslinking is achieved. Importantly, we elucidate the mechanism in depth and show that the MP-CR strategy can comprehensively improve the overall performance of natural hierarchical materials. The MP-CR strategy represents a significant step forward for the internal modification of hierarchical materials, which will find broad applications in biomedicine, catalysis, water treatment, soft electronics, and energy storage.