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HighlightsTwo functionally different anisotropic layers are rationally assembled for highly selective and stretchable multidirectional strain sensors.    Concurrently excellent selectivity, sensitivity, stretchability, and linearity up to 100% strain is demonstrated for the first time in a multidirectional strain sensor.    A novel stepwise crack propagation mechanism is proposed to enable high stretchability and linearity.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-021-00615-5.

Anisotropic, Wrinkled, and Crack-Bridging Structure for Ultrasensitive, Highly Selective Multidirectional Strain Sensors