AbstractOrganic phototransistors can enable many important applications such as nonvolatile memory, artificial synapses, and photodetectors in next‐generation optical communication and wearable electronics. However, it is still a challenge to achieve a big memory window (threshold voltage response ∆Vth) for phototransistors. Here, a nanographene‐based heterojunction phototransistor memory with large ∆Vthresponses is reported. Exposure to low intensity light (25.7 µW cm−2) for 1 s yields a memory window of 35 V, and the threshold voltage shift is found to be larger than 140 V under continuous light illumination. The device exhibits both good photosensitivity (3.6 × 105) and memory properties including long retention time (>1.5 × 105s), large hysteresis (45.35 V), and high endurance for voltage‐erasing and light‐programming. These findings demonstrate the high application potential of nanographenes in the field of optoelectronics. In addition, the working principle of these hybrid nanographene‐organic structured heterojunction phototransistor memory devices is described which provides new insight into the design of high‐performance organic phototransistor devices.