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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 …