“…Such soft molecular crystals shatter the preconceived notion that crystals are brittle and hard and, when struck or bent with external force, they typically crack or shatter, inevitably. , The soft matter of organic single crystals responds to external force in a different manner: they show plastic or elastic deformation . These soft molecular crystals share properties of both crystals and soft matter, endowing them with great potential in mechanical actuators, optical devices, − organic electronics, etc. − The mechanical properties of molecular crystals strongly rely on the molecular packing arrangements and intermolecular interactions, which can be tailored by crystal engineering approaches. − Designing new structures with the desired physical and chemical properties using advanced third-generation strategies of crystal engineering is an attractive and rapidly developing research area. , Much effort has been made to study the mechanism of flexible crystals and gain a deep understanding of mechanical compliance to a large extent. − The importance of weak dispersive interactions has been acknowledged as it has a natural advantage in controlling local molecular movements, which is essential to ensure the effective dissipation of stresses generated from structural functions. Almost all of the key structures of mechanically flexible crystals exhibit a combination of weak intermolecular interactions such as van der Waals (vdW), weak hydrogen-bonding, , lighter halogen, ,, and π···π interactions. , Several recent studies reported unusual plastic crystals based on strong hydrogen bonding. , Strong hydrogen bonding was also found to play a nonnegligible role in elastic crystals of isosorbide 5-mononitrate and (2 S ,3 R )-3-ethyl-1-phenylhex-5ene-2,3-diol .…”