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Neuromorphic computing systems that are capable of parallel information storage and processing with high area and energy efficiencies, offer important opportunities for future storage systems and in‐memory computing. Here, it is shown that a carbon dots/silk protein (CDs/silk) blend can be used as a light‐tunable charge trapping medium to fabricate an electro‐photoactive transistor synapse. The synaptic device can be optically operated in volatile or nonvolatile modes, ensuring concomitant short‐term and long‐term neuroplasticity. The synaptic‐like behaviors are attributed to the photogating effect induced by trapped photogenerated electrons in the hybrid CDs/silk film which is confirmed with atomic force microscopy based electrical techniques. In addition, system‐level pattern recognition capability of the synaptic device is evaluated by a single‐layer perceptron model. The remote optical operation of …