CNT‐induced formation of transcrystals of γ‐PP are reported. Formation of these transcrystals occurred when PP was infiltrated into nanotube aerogel fibers to form polymer nanocomposites. The PP morphology and microstructure with particular focus on the interfacial region of the CNTs were investigated by means of SEM, DSC and WAXD. The transcrystalline supramolecular microstructures were observed around the individual nanotubes during quiescent melting crystallization. Microstructural analysis showed that γ‐form transcrystals of PP dominate the overall interfacial structure. The content of γ‐form transcrystals increased with increase in nanotube loading. The mechanical properties and electrical conductivities of the nanocomposites have been evaluated.magnified image