Large-strain fl exible sensors have been developed via combining elastic substrate (e.g., silicone elastomer) with a rigid sensing material such as nanocarbons (e.g., nanotubes [ 4,5 ] and graphene [ 6,7 ] ), metal nanowires, [ 3 ] conducting polymers [ 8 ] and piezoelectric materials, [ 9 ] through surface attachment, interlayer lamination or blending. [ 2,4,7,10 ] For example, Yamada et al. [ 4 ] prepared a strain sensor by depositing single-walled carbon nanotubes onto a polydimethylsiloxane fi lm. The sensor had a strain detection range of 0-280%, which was 50 times larger than that of conventional metal strain gauges.Fibrous materials such as yarn, [ 11 ] woven fabric, [ 12,13 ] nonwoven fi ber mat, [ 14,15 ] and electrospun fi ber membrane [ 15,16 ] have been shown great advantages in developing fl exible strain sensors. They have excellent structure stability, deformation recoverability, permeability to air/moisture and porosity, promising as substrate for wearable sensors. Mattmann et al. [ 17 ] prepared a strain sensor by incorporating a conducting fi ber, which was made of a copolymer and carbon black into a textile.Flexible sensors capable of detecting large strain are very useful for health monitoring and sport applications. Here a strain sensor is prepared by applying a thin layer of conducting polymer, polypyrrole (PPy), onto the fi ber surface of an elastic fi brous membrane, electrospun polydimethylsiloxane (PDMS). The sensor shows a normal monotonic resistance response to strain in the range of 0-50%, but the response becomes "on-off switching" mode when the strain is between 100 and 200%. Both response modes are reversible and can work repeatedly for many cycles. This unique sensing behavior is attributed to overstretching of the polypyrrole coating, unique fi brous structure, and elasticity of PDMS fi bers. It may be useful for monitoring the states where motions are only allowed in a particular range such as joint rehabilitation.