© 2017 Wiley Periodicals, Inc. The electrical, mechanical, and piezoresistive properties of ternary composites based on elastomeric polydimethylsiloxane (PDMS), carbon nanotubes (CNTs), and polyaniline (PANI) were studied and compared with those of binary PDMS–CNT composites. The presence of PANI affected the percolating network of the CNTs. At lower PANI concentrations (2.5 and 5%), the conductive network of the CNTs was constructively modified; this led to an enhancement in the conductivity in the sample containing 2% CNTs. A higher PANI content (7.5%) hindered the flow of main charge carriers through the composite. The piezoresistive response of the binary and ternary composites was studied by cyclic experiments under compression loads. In all of the samples, the electrical resistance increased monotonically up to a 10% strain. The reproducibility of the piezoresistive behavior in the binary and ternary composites provided evidence that the fillers could reversibly recover their initial position together with the PDMS chains without a significant displacement with respect to their original positions. The reduction of the piezoresistive sensibility by PANI addition was attributed to the displacement restrictions of the CNTs within the composite under pressure because of the volume exclusion of PANI particles; this maintained the probability of CNT contact and increased the possibility of the formation of new CNT conductive channels. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 44780.