Hydrogels are ideal candidates for various advanced applications, including wearable electronics, soft robots, and biomedical engineering, which benefit from their natural merits of softness, deformability, and biocompatibility. In the early stages since the emergence of hydrogels, tremendous efforts have been made to improve their mechanical performances. Despite the investigation of several mechanical strengthening strategies, including nanocomposites, noncovalent cross-linking, and topological design, single network hydrogels still grapple with the trade-off between mechanical strength and functionality. As a result, improving network complexity and functional diversification have emerged as a significant trend in gel development. Multiphase gels are developed to incorporate mechanical enhancement components and functional components, obtaining integrated exceptional performances. This Account seeks to review mechanical strength-function integrated gels fabricated by bioinspired multiphase confinement strategy, providing inspiration and guidance for multiphase gel design. The first part starts with a specific elaboration on bioinspired strategy, involving tissue structure analysis, biological mechanism imitation, and bioinspired materials fabrication. By exploring human skeletal muscle and nacre, we elucidate how to connect biological structures and artificial material design concretely. Meanwhile, we highlight the promotion effect of in-depth analysis on the biological micro structure and working mechanism. In the next part, we subsequently evaluate diverse multiphase network structures that were previously developed and showcase their exceptional performances and unique applications. Multiple gels developed by our group─phase separation ionic gels for stiffness changing materials, phase transition organohydrogels for actuation, interpenetrating organohydrogels for lubrication, etc.─are reviewed in this section. The most crucial point for the fabrication of these multiphase gels is stability, which inextricably links to their interface interactions. Therefore, we summarize the techniques employed to establish ultrastable interfaces, such as emulsion interface interaction or heterogeneous interpenetrating networks. We delve into the manifold network structures of multiphase polymers, encompassing plasticity, elasticity, hydrophilicity, and hydrophobicity. Different fabrication strategies were adopted according to their network properties, with the aim of exhibiting their unique mechanical strength and functions. In these confined multiphase structures, the independent motions of orthogonal networks are achieved. Additionally, polymers confined in space in nanometer scale or smaller can exhibit performances deviated from bulk phase, including crystallinity, alignment degree, and glass transition temperature. The discussion also covers the confinement effects on the polymer structure and mobility. Ultimately, we introduce the advanced applications of multiphase gels, spanning broad areas including lubrication, actuation, mechanical adaptation, soft robotics, sensing, etc. In order to look into the future development direction of multiphase hydrogels, we derive conclusions about their challenges and opportunities.

中文翻译：

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使用空间限制策略的仿生多相凝胶

水凝胶是各种先进应用的理想选择，包括可穿戴电子产品、软机器人和生物医学工程，这些应用得益于其柔软性、可变形性和生物相容性的天然优点。自水凝胶出现以来的早期阶段，人们为提高其机械性能付出了巨大的努力。尽管研究了几种机械强化策略，包括纳米复合材料、非共价交联和拓扑设计，但单网络水凝胶仍然难以在机械强度和功能之间进行权衡。因此，提高网络复杂性和功能多样化已成为凝胶开发的重要趋势。开发多相凝胶以结合机械增强成分和功能成分，获得综合的卓越性能。本报告旨在回顾通过仿生多相限制策略制造的机械强度功能集成凝胶，为多相凝胶设计提供灵感和指导。第一部分首先具体阐述仿生策略，包括组织结构分析、生物机制模拟和仿生材料制造。通过探索人体骨骼肌和珍珠质，我们阐明了如何具体连接生物结构和人造材料设计。同时，我们突出了深入解析生物微观结构和工作机制的促进作用。在下一部分中，我们随后评估先前开发的各种多相网络结构，并展示其卓越的性能和独特的应用。本节对我们课题组开发的多种凝胶——用于改变刚度材料的相分离离子凝胶、用于驱动的​​相变有机水凝胶、用于润滑的互穿有机水凝胶等进行综述。制造这些多相凝胶的最关键点是稳定性，这与它们的界面相互作用密不可分。因此，我们总结了用于建立超稳定界面的技术，例如乳液界面相互作用或异质互穿网络。我们深入研究多相聚合物的多种网络结构，包括塑性、弹性、亲水性和疏水性。根据其网络特性采用不同的制造策略，以展示其独特的机械强度和功能。在这些受限多相结构中，实现了正交网络的独立运动。此外，限制在纳米级或更小空间内的聚合物可能表现出偏离体相的性能，包括结晶度、取向度和玻璃化转变温度。讨论还涵盖了对聚合物结构和迁移率的限制效应。最终，