Simple methods for patterning single crystals are critical to fully realize their applications in electronics. However, traditional vapor and solution methods are deficient in terms of crystals with random spatial and quality distributions. In this work, we report a dewetting-induced assembly strategy for obtaining large-scale and highly oriented organic crystal arrays. We also demonstrate that organic field-effect transistors (OFETs) fabricated from patterned n-alkyl-substituted tetrachloroperylene diimide (R–4ClPDI) single crystals can reach a maximum mobility of 0.65 cm2 V–1 s–1 for C8–4ClPDI in ambient conditions. This technique constitutes a facile method for fabricating OFETs with high performances for large-scale electronics applications. ACS Appl. Mater. Interfaces,2016 |