The p-type properties of carbon nanotubes (CNTs) in organic thermoelectric devices need urgent improvement for large-scale, low-grade thermal energy applications. Here, we present a suitable approach to significantly enhance the power factor (PF) by increasing the electrical conductivity through the low-temperature calcination-induced pyrolysis of the insulating γ-cyclodextrin polymer (PγCyD), which is used as a solubilizer of film-like CNTs. The low-temperature calcination method, which can be used to realize good electrical contact between CNT bundles, shows enhancement behavior as a universal phenomenon for not only PγCyD but also other commonly used polymers for CNT films. To moderate the calcination temperature, the Pd catalyst was added, and the optimal temperature was reduced from 340 °C to 250 °C. Consequently, the PF value of the CNT film was 570 μW m−1 K−2, which was found to be more than twice that of the original CNT film. In addition, we demonstrated the energy harvesting capability of a thermoelectric generator based on this p-type CNT film; a thermoelectric generator with 10 p-type thermoelectric elements showed a maximum power output of 10.3 μW with a temperature difference of 75 °C, which is comparable to the maximum power output of some of the best single-component organic thermoelectric devices demonstrated to date. This outstanding output power shows that easy-to-handle CNT films with low-temperature heat treatment can open new avenues for the development of thermoelectric generators.

The fabrication of low-temperature waste heat power conversion modules will require the development of thermoelectric materials based on mass-produced nanotubes such as super-growth carbon nanotubes (SGCNTs), rather than high-quality nanotubes generated on the laboratory scale. In this work, SGCNT films co-loaded with colloidal ZnO (which has a high Seebeck coefficient) and Ag (which enhances electrical conductivity) were prepared to optimize both carrier concentration and mobility. The resulting carbon-based hybrid films were found to have a p-type power factor of 100.4 µW m −1 K −2 at 383 K, which represented one of the highest values yet reported for a SGCNT system.