Flexible strain sensors have been widely used in many fields because of their excellent adaptability and flexibility. Nonetheless, creating these sensors through simple methods that achieve a low percolation threshold and high sensitivity continues to pose a challenge. In this paper, a segregated structure was realized in a carbon nanotube/polydimethylsiloxane (CNT/PDMS‐S) strain sensor by a sustainable emulsion method that involved the mixing cellulose nanocrystals (CNCs), CNTs, PDMS and water. The incorporation of CNC improved the stability of CNTs in aqueous suspension. Consequently, The CNT@CNC nanocomposites were strategically placed in the gaps between the PDMS microspheres, creating a segregated structure. The segregated structure notably lowered the percolation threshold of the composite to 0.49 wt%. Moreover, we found that the CNT/PDMS‐S sensor containing 1.5 wt% CNTs showed excellent sensing performance, which not only had a wide strain measurement range and could adapt to the strain change from 0% to 70%, but also had high sensitivity with a gauge factor (GF) of 290 at 70% strain. Meanwhile, the sensor had an excellent linear response (R2 ≥ 0.96) and can monitor the minimum strain of 0.1%. The proposed sensor demonstrated excellent response when applied to sense wrist movement, facial movement and closure, and syllable recognition.Highlights
Strain sensors with a segregated structure were realized by a sustainable method.
The segregated structure greatly reduces the percolation threshold of sensor.
The sensor has a high sensitivity, linearity, and wide strain detection range.
The sensor features high resolution for tiny deformations sensing.