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Atomically thin materials such as graphene are uniquely responsive to charge transfer from adjacent materials, making them ideal charge‐transport layers in phototransistor devices. Effective implementation of organic semiconductors as a photoactive layer would open up a multitude of applications in biomimetic circuitry and ultra‐broadband imaging but polycrystalline and amorphous thin films have shown inferior performance compared to inorganic semiconductors. Here, the long‐range order in rubrene single crystals is utilized to engineer organic‐semiconductor–graphene phototransistors surpassing previously reported photogating efficiencies by one order of magnitude. Phototransistors based upon these interfaces are spectrally selective to visible wavelengths and, through photoconductive gain mechanisms, achieve responsivity as large as 10 7  A W −1  and a detectivity of 9 × 10 11  Jones at room temperature. These findings point toward implementing low‐cost, flexible materials for amplified imaging at ultralow light levels.

Highly Efficient Rubrene–Graphene Charge‐Transfer Interfaces as Phototransistors in the Visible Regime