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Abstract The application of hardware‐based neural networks can be enhanced by integrating sensory neurons and synapses that enable direct input from external stimuli. This work reports direct optical control of an oscillatory neuron based on volatile threshold switching in V₃O₅. The devices exhibit electroforming‐free operation with switching parameters that can be tuned by optical illumination. Using temperature‐dependent electrical measurements, conductive atomic force microscopy (C‐AFM), in situ thermal imaging, and lumped element modelling, it is shown that the changes in switching parameters, including threshold and hold voltages, arise from overall conductivity increase of the oxide film due to the contribution of both photoconductive and bolometric characteristics of V₃O₅, which eventually affects the oscillation dynamics. Furthermore, V₃O₅is identified as a new bolometric material with a temperature coefficient of resistance (TCR) as high as −4.6% K⁻¹at 423 K. The utility of these devices is illustrated by demonstrating in‐sensor reservoir computing with reduced computational effort and an optical encoding layer for spiking neural network (SNN), respectively, using a simulated array of devices.