Аннотация:Organic electronics is a rapidly developing high‐tech area aimed at production of electronic devices that can outperform traditional inorganic ones in many applications. However, in contrast to inorganic semiconductors, organic ones are “soft” materials – they consist of molecules bound by weak non‐covalent forces. The weakness of the intermolecular interaction in organic semiconductors makes the charge mobility – the key figure‐of‐merit for charge transport – very sensitive to the intra‐ and intermolecular vibrations, which tend to localize charge carriers at a single molecule via electron‐phonon interaction. In this chapter, we review computational and experimental approaches for description of the intra‐ and intermolecular vibrations of organic semiconductor crystals (OSCs) – the class of organic semiconductors showing the highest charge mobility – and impact of these vibrations on charge transport. We focus on the low‐frequency vibrations, which are believed to limit the charge mobility in high‐mobility OSCs but remain a challenge for theoretical description. The dramatical impact of the number of independent molecules in the OSC unit cell on the low‐frequency vibrational spectrum and electron‐phonon interaction is highlighted. The results presented are important for a focused search of OSCs with suppressed negative impact of vibrations on charge transport and hence potentially high charge mobility.