Covalent Organic Frameworks In article number 2304989, Lei-Lei Liu, Zhongyue Li, and co-workers synthesize a calix[4]arene-derived covalent organic framework (COF)-C4A-benzothiadiazole (BTD), which exhibits high crystallinity and features a non-interpenetrating undulating 2D layered structure with AA-stacking. COF-C4A-BTD has an appropriate electron donor-acceptor and energy band structures which can facilitate the generation and separation of ·O2− and h+, resulting in efficient visible-light-driven activity for degrading Bisphenol A, Rhodamine B, and Methylene blue.