Direct crystallization of polymer crystals along the long axis of carbon nanotubes (CNTs) to produce a hybrid nanostructured material is expected to retain the properties of CNTs and has the advantage of a strong polymer/CNT interface. Three different polymer systems are selected to elucidate the fundamental principles that govern the processing of organic–inorganic hybrid nanostructured materials with nanometer‐scale architecture. The tunable character of the nanometer‐scale hybrid architecture is investigated as a function of undercooling and polymer concentration. It is observed that while polyethylene and nylon 6,6 crystallize in a periodic manner as disk‐shaped crystals along the long axis of the CNTs, the polypropylene–CNTs result in conventional spherulites. The reasons for these differences are analyzed.

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