Designing a crosslinked polymer with autonomous self-healing at room temperature (RT) remains an arduous challenge because the topological network reconstructions are governed by crosslinking. Herein, a flexible strategy is described to develop intrinsically dynamic crosslinked elastomers with RT self-healing via a photo-initiated copolymerization to address these issues. The key is to incorporate a urea–urethane structure with dynamic urea bond into the polymer network as a flexible crosslinking unit. This strategy endows the crosslinked elastomer with superior properties, including autonomously rapid self-healing at RT, extreme stretchability of up to 1726%, high toughness (∼24.45 MJ m^–3), extended stability, and recyclability. Upon damaged, the resultant elastomers instantly self-heal at RT and completely self-heal within 10 min without the assistance of external triggers. These amazing properties of the dynamic elastomer are attributed to the synergistic effect of the robustly dynamic urea bonds and inter- and intrachain hydrogen bond interactions. Notably, the self-healing and mechanical properties of the network can be optimized by tuning the dynamic crosslinker content. Dynamic reversibility occurs at RT evidenced by rheological tests. The facile fabrication method and multifunctional properties of the self-healable and stretchable crosslinked elastomer demonstrate that it shows great potential in smart protective coating and wearable electronics industry.

设计在室温（RT）下具有自发自愈能力的交联聚合物仍然是一项艰巨的挑战，因为拓扑网络的重建受交联的支配。在本文中，描述了一种灵活的策略，可以通过光引发的共聚反应开发具有RT自修复功能的内在动态交联弹性体，以解决这些问题。关键是将具有动态尿素键的尿素-尿烷结构纳入聚合物网络中，作为柔性交联单元。这种策略赋予了交联弹性体以优异的性能，包括在RT时自动快速自我修复，高达1726％的极高可拉伸性，高韧性（〜24.45 MJ m ^–3），扩展的稳定性和可回收性。损坏后，所得的弹性体可在室温下立即自我修复，并在10分钟内完全自我修复，而无需外部触发器的帮助。动态弹性体的这些惊人性能归因于强大的动态尿素键以及链间和链内氢键相互作用的协同效应。值得注意的是，可以通过调整动态交联剂的含量来优化网络的自我修复和机械性能。流变学测试证明，RT时发生动态可逆性。自修复和可拉伸交联弹性体的简便制造方法和多功能特性表明，它在智能保护涂层和可穿戴电子行业中显示出巨大的潜力。