Chem. Sci., 2025, Advance Article DOI: 10.1039/D5SC03645C, Edge Article Tiancun Liu, Xiao-Meng Lu, Song Lu, Ronghan Jiang, Min Guo, Chaofei Guo, Zhixin Yu, Yong Wang Lithiophilic imine-based covalent organic frameworks (ICOFs) with built-in silver (Ag) sites (Ag@ICOFs) are demonstrated to effectively guide dendrite-free lithium deposition.