A Microporous Hydrogen‐Bonded Organic Framework with Open Pyrene Sites Isolated by Hydrogen‐Bonded Helical Chains for Efficient Separation of Xenon and Krypton

/g, with an Xe/Kr IAST selectivity of 22.0; both values surpass those of currently known top-performing HOFs. Breakthrough experiments confirmed its superior separation performance with a separation factor of 8.6 and a yield of high-purity Kr (>99.5 %) of 184 mL/g. Furthermore HOF-FJU-168 exhibits excellent thermal and chemical stability, as well as renewability. Single-crystal X-ray diffraction and molecular modeling revealed that the unique electrostatic surface potential around the open pyrene sites creates a micro-electric field, exerting a stronger polarizing effect on Xe than on Kr, thereby enhancing host-Xe interactions.