Abstract Nanoparticle embedded carbon nanotube papers can produce flexible functional films, whose function is based on the electronic coupling of the nanoparticles with the network of carbon nanotubes. Here we report on the expansion of a synergistic light-free catalyst system that requires both the molecular wire capability of multi-walled carbon nanotubes and the piezoelectric properties of ZnO nanoparticles. The electron–hole pairs can be induced by the piezoelectric effect of ZnO nanoparticles under the effect of pressure. The strong oxidizing radicals interact with the electron–hole pairs and aqueous solution to induce the degradation of methylene blue without the requirement of light. This study highlights the use of nanoparticles for the piezoelectric – light free catalyst system and the limitations of increased nanoparticle loading on the catalytic degradation of methylene blue.