Cryo‐electron diffraction tomography (Cryo‐EDT) has been developed to determine the crystal structures of covalent organic frameworks (COFs) and their host‐guest interaction at the atomic precision, whose crystals are only submicron‐sized, organic, porous, and dynamic. The keys of 3D electron diffraction (3D‐ED) techniques are low‐dose beam, sample cryo‐handling, fast data collection, sensitive detector, and direct space structure solution. We envision the development of COF chemistry will be propelled by such powerful 3D‐ED techniques for a better understanding at the molecular level and correlation of structures to chemicophysical properties. More details are discussed in the article by Zhang et al. on page 1153—1166.
