LAUSR

Organic single‐crystal films (OSCFs) provide an unprecedented opportunity for the development of new‐generation organic single‐crystal electronics. However, crystallization of organic films is normally governed by stochastic nucleation and incoherent growth, posing a formidable challenge to grow large‐sized OSCFs. Here, an “orientation filter funnel” concept is presented for the scalable growth of OSCFs with well‐aligned, singly orientated crystals. By rationally designing solvent wetting/dewetting patterns on the substrate, this approach can produce seed crystals with the same crystallographic orientation and then maintain epitaxial growth of these crystals, enabling the formation of large‐area OSCFs. As a result, this unique concept for crystal growth not only enhances the average mobility of organic film by 4.5‐fold but also improves its uniformity of electrical properties, with a low mobility variable coefficient of 9.8%, the new lowest record among organic devices. The method offers a general and scalable route to produce OSCFs toward real‐word electronic applications.