To optimize the structure of the flexible piezoresistive sensor based on conductive polymer composite and widen the workable pressure range, a piezoresistive sensor with a multilayered structure based on carbon nanotubes/carbon black/silicone rubber conductive composite was designed and investigated. Different from the traditional monolayer structure, this novel multilayered sensor consisted of three microstructured piezoresistive composite films. The experimental data showed that the electrical resistance of the sensor varied regularly with a wide range of applied pressure (0–1.8 MPa at least). The high sensitivity, high flexibility, facile fabrication, and low cost were also the advantages of this pressure sensor. In addition, the piezoresistive mechanism was studied and shown to be the synergistic effects of the contact resistance mechanism and bulk resistance mechanism. Factors influencing the piezoresistive properties were also investigated. Moreover, the consecutive loading tests verified the feasibility and stability to use this sensor element for pressure measurement.
