Multiscale integral synchronous assembly of cuttlebone-inspired structural materials by predesigned hydrogels

Huai-Bin Yang; Yi-Xing Lu; Xin Yue; Zhao-Xiang Liu; Wen-Bin Sun; Wen-Pei Zheng; Qing-Fang Guan; Shu-Hong Yu

doi:10.1038/s41467-024-55344-1

Multiscale integral synchronous assembly of cuttlebone-inspired structural materials by predesigned hydrogels

Nat Commun. 2025 Jan 2;16(1):62. doi: 10.1038/s41467-024-55344-1.

Authors

Huai-Bin Yang^#¹, Yi-Xing Lu^#¹, Xin Yue^#¹, Zhao-Xiang Liu¹, Wen-Bin Sun¹, Wen-Pei Zheng¹, Qing-Fang Guan², Shu-Hong Yu^{3

4}

Affiliations

¹ Department of Chemistry, New Cornerstone Science Institute, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China.
² Department of Chemistry, New Cornerstone Science Institute, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China. guanqf@ustc.edu.cn.
³ Department of Chemistry, New Cornerstone Science Institute, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China. shyu@ustc.edu.cn.
⁴ Institute of Innovative Materials (I2M), Department of Materials Science and Engineering, Department of Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China. shyu@ustc.edu.cn.

^# Contributed equally.

Abstract

The overall structural integrity plays a vital role in the unique performance of living organisms, but the integral synchronous preparation of different multiscale architectures remains challenging. Inspired by the cuttlebone's rigid cavity-wall structure with excellent energy absorption, we develop a robust hierarchical predesigned hydrogel assembly strategy to integrally synchronously assemble multiple organic and inorganic micro-nano building blocks to different structures. The two types of predesigned hydrogels, combined with hydrogen, covalent bonding, and electrostatic interactions, are layer-by-layer assembled into brick-and-mortar structures and close-packed rigid micro hollow structures in a cuttlebone-inspired structural material, respectively. The cuttlebone-inspired structural materials gain crack growth resistance, high strength, and energy absorption characteristics beyond typical energy-absorbing materials with similar densities. This hierarchical hydrogel integral synchronous assembly strategy is promising for the integrated fabrication guidance of bioinspired structural materials with multiple different micro-nano architectures.