In this work, the influence of the material of the contact sublayer and the growth temperature on the geometric dimensions and the value of the piezoelectric response of carbon nanotubes for their use in nanopiezotronic devices is investigated. The thermodynamic laws that characterize the processes occurring in the "catalyst/sublayer/substrate" system have been established. It was found that with an increase in temperature, the carbon nanotubes density decreases from 1.1 to 0.001 µm−2 for Mo, and from 26 to 0.1 µm−2 for Cr. The value of the piezoelectric response was estimated, which ranged from 8 to 14 nA for the Cr sublayer and from 3 to 23 nA for the Mo sublayer. It is shown that the obtained structures are promising for the creation of nanopiezotronic elements (nanogenerators, energy nanoharvesters).