Nanocomposites of carbon nanotube fibers have been prepared using controlled polymer crystallization confined in nanotube aerogel fibers. The polyethylene nanocomposites have been investigated by means of polarized optical microscopy (POM), scanning electron microscopy (SEM) and wide-angle X-ray diffraction (WAXD). The individual nanotubes are periodically decorated with polyethylene nanocrystals, forming aligned hybrid shish-kebab nanostructures. After melting and recrystallization, transcrystalline lamellae connecting the adjacent aligned nanotubes develop. Microstructural analysis shows that the nanotubes can nucleate the growth of both orthorhombic and monoclinic crystals of polyethylene in the quiescent state. The tensile strength, modulus, and axial electrical conductivity of these polyethylene/CNT composite fibers are as high as 600 MPa, 60 GPa, and 5000 S/m, respectively.