Different polymer matrices (polyisoprene, ethylene-vinyl acetate etc.) and various electroconductive nanosized carbon allotropes (carbon black (CB), carbon nanotubes) were used to elaborate composites for multifunctional sensing. The carbon allotrope fillers were used in two ways – as one separate allotrope, and as two allotrope mix (hybrid). An attempt to increase the performance of chemical sensing was made by aligning of the conductive nanoparticles in liquid matrix using DC as well as AC electric field (Figure 1a). The obtained polymer/nanostructured carbon composites (PNCC) possess piezoresistivity. The composites showed positive pressure coefficient of resistance – the resistance increases with increasing compressive force. By combining separate layers of PNCC in specific structure a sample with negative pressure coefficient of resistance (when the resistance decreases with increasing compressive force) was elaborated. For the first time uncommon piezopermittivity effect was found – the real part of permittivity of PNCC noticeably decreases as pressure is applied (Figure 1b). A supercapacitor that was elaborated using porous PNCC as electrodes for the first time was tested as a pressure indicator and an enhanced piezopermittivity effect was found. In the latter case, as pressure was applied, the permittivity increased. Planar design PNCC responds to concentration changes of volatile organic compounds (Figure 1a) as well as humidity changes in surrounding environment. Triboelectric nanogenerators with PNCC components were also elaborated and tested as pressure indicators, where the mechanical vibrations induce the periodical voltage changes. The PNCC with positive temperature coefficient showed photothermal response to laser radiation – the electrical resistance changed in opposite way compared to common semiconductor photodetectors. The mechanism of each sensing effect is explained basing mainly on quantum charge tunneling effect between adjacent nanoparticles in percolative conductive channel structure inside the polymer matrix.