Field-effect transistors based on single crystals of organic semiconductors have the highest reported charge carrier mobility among organic materials, demonstrating great potential of organic semiconductors for electronic applications. However, single-crystal devices are difficult to fabricate. One of the biggest challenges is to prepare dense arrays of single crystals over large-area substrates with controlled alignment. Here, we describe a solution processing method to grow large arrays of aligned C60 single crystals. Our well-aligned C60 single-crystal needles and ribbons show electron mobility as high as 11 cm2V–1s–1 (average mobility: 5.2 ± 2.1 cm2V–1s–1 from needles; 3.0 ± 0.87 cm2V–1s–1 from ribbons). This observed mobility is ∼8-fold higher than the maximum reported mobility for solution-grown n-channel organic materials (1.5 cm2V–1s–1) and is ∼2-fold higher than the highest mobility of any n-channel organic material (∼6 cm2V–1s–1). Furthermore, our deposition method is scalable to a 100 mm wafer substrate, with around 50% of the wafer surface covered by aligned crystals. Hence, our method facilitates the fabrication of large amounts of high-quality semiconductor crystals for fundamental studies, and with substantial improvement on the surface coverage of crystals, this method might be suitable for large-area applications based on single crystals of organic semiconductors.