Fullerene (C 60 ) single crystals with exceptionally low defects and nearly perfect translational symmetry make them appealing in achieving high-performance n-type organic transistors. However, because of its natural 0D structure, control over continuous crystallization of C 60 over a large area is extremely challenging. Here, the authors report a solution-phase epitaxial approach for wafer-scale growth of continuously aligned C 60 single crystals. This method enables the rational control of the density of nucleation event at meniscus front by confining the size and shape of meniscus with a microchannel template. In this case, a single nucleus as seed crystal can be formed at the front of meniscus, and then epitaxial growth from the seed crystal occurs with continuous retreat of the meniscus. As a result, highly uniform C 60 singlecrystal array with ultralow defect density is obtained on 2-inch substrate. Organic field-effect transistors made from the C 60 single-crystal array show a high average electron mobility of 2.17 cm 2 V −1 s −1 , along with a maximum mobility of 5.09 cm 2 V −1 s −1 , which is much superior to the C 60 polycrystalline film-based devices. This strategy opens new opportunities for the scalable fabrication of high-performance integrated devices based on organic crystals.