Electrical Percolation and Piezoresistive Response of Vulcanized Natural Rubber/MWCNT Nanocomposites

A flexible piezoresistive material based on vulcanized natural rubber (VNR) and multiwalled carbon nanotubes (MWCNTs) was developed and systematically investigated for strain sensing applications. The nanocomposites were prepared by melting and vulcanizing MWCNT, while keeping the rubber composition constant to isolate the effect of the conductive nanofiller. By scanning electron microscopy, morphological analyses indicated that MWCNTs were dispersed throughout the rubber matrix, with localized agglomerations becoming more evident at higher loadings. In mechanical tests, MWCNT incorporation increases the tensile strength of VNR, increasing the stress at break from 8.84 MPa for neat VNR to approximately 10.5 MPa at low MWCNT loadings. According to the electrical characterization, VNR-MWCNT nanocomposite exhibits a strong insulator–conductor transition, with the electrical percolation threshold occurring between 2 and 4 phr. The dc electrical conductivity increased sharply from values on the order of 10−14 S·m−1 for neat VNR to approximately 10−3 S·m−1 for nanocomposites containing 7 phr of MWCNT. Impedance spectroscopy revealed frequency-independent conductivity plateaus above the percolation threshold, indicating continuous conductive pathways, while dielectric analysis revealed strong interfacial polarization effects at the MWCNT–VNR interfaces. The piezoresistive response of samples containing MWCNT exhibited a stable, reversible, and nearly linear response under cyclic tensile deformation (10% strain). VNR/MWCNT nanocomposites demonstrate mechanical compliance and tunable electrical sensitivity, making them promising candidates for flexible and low-cost piezoresistive sensors.