The development of photostimulated‐motion artificial reflex arcs — a neural circuit inspired by light‐driven motion reflexes — holds significant promises for advancements in robotic perception, navigation, and motion control. However, the fabrication of such systems, especially those that accommodate multiple actions and exhibit gradient responses, remains challenging. Here, we developed a gradient‐responsive photostimulated‐motion artificial reflex arc by integrating a programmable and tunable photoreceptor based on folded MoS2 at different twist angles. The twisted folded bilayer MoS2 used as photoreceptors could be customized via the transfer technique using patternable paraffin, where the twist angle and fold‐line could be controlled. The photoluminescence (PL) intensity was 3.7 times higher at a twist angle of 29° compared to that at 0°, showing a monotonically decreasing indirect bandgap. Through tunable interlayer carrier transport, photoreceptors fabricated using folded bilayer MoS2 at different twist angles demonstrated gradient response time, enabling the photostimulated‐motion artificial reflex arc for multi‐action responses. They were transformed to digital command flow and studied via machine learning to control the gestures of a robotic hand, showing a prototype of photostimulated gradient‐responsive artificial reflex arcs for the first time. Our work provides a unique idea for developing intelligent soft robots and next‐generation human‐computer interfaces.This article is protected by copyright. All rights reserved