Ultralong organic phosphorescence (UOP) crystals have attracted increased attention due to the distinct photophysical property of a long-lived lifetime. However, organic crystals are generally brittle, leading to a serious problem for their application in flexible technology. Herein, we report three types of elastic organic crystals (EOCs) with ultralong phosphorescence via introducing halogen atoms (Cl, Br, I) into π-conjugated phosphorescent molecules. Especially, the crystal containing iodine atoms displayed both excellent elasticity (ε = 3.01%) and high phosphorescent efficiency (Φ_Ph = 19.1%) owing to the strong halogen bonds. Taking advantage of its highly efficient UOP and excellent elasticity, we successfully used a DCz4I crystal for anti-counterfeiting application. These findings may provide guidance for the development of elastic crystals with afterglow and expand the scope of potential applications on flexible materials.

由于长寿命的独特光物理特性，超长有机磷光 (UOP) 晶体引起了越来越多的关注。然而，有机晶体普遍较脆，导致其在柔性技术中的应用存在严重问题。在此，我们通过将卤素原子（Cl、Br、I）引入 π 共轭磷光分子，报告了三种具有超长磷光的弹性有机晶体（EOC）。特别是，含有碘原子的晶体同时显示优异的弹性（ε  = 3.01％）和高的磷光效率（Φ_博士 = 19.1%）由于强卤键。利用其高效的UOP和出色的弹性，我们成功地将DCz4I晶体用于防伪应用。这些发现可能为开发具有余辉的弹性晶体提供指导，并扩大在柔性材料上的潜在应用范围。