LAUSR

Metallic two‐dimensional conductive nanomaterials are extensively explored in stretchable strain sensors, which have promising applications ranging from health monitoring to human–machine manipulation. However, there are limited materials available in this category, and their sensing abilities need to be strengthened. Herein, a controllable deoxidation–nitridation strategy via the pyrolysis of an amine nitrogen source to synthesize oxygen‐doped vanadium nitride (VNO) nanosheets with high conductivity is reported. Its metallic characteristics and low dimensionality, together with layer‐to‐layer slippage make VNO particularly suitable for stretchable strain sensors with remarkable performance, including extraordinary sensitivity (a maximum gauge factor of 2667), wide detection range (0–100%), high durability (over 6000 cycles), and rapid response (44 ms). Furthermore, the strain sensors can capture various physiological signals; in particular, a state‐of‐the‐art wireless vehicle control system designed for differently abled people is fabricated based on the sensors. Moreover, by engineering the thickness of the VNO layer, it can behave as an elastic conductor, demonstrating its feasibility for stretchable wiring.