Sheets of aligned multi-walled carbon nanotubes (AMWCNTs) were used to study the structural annealing of pyrolytic carbon (PyC) coatings with various thicknesses on MWCNTs. PyC was deposited using chemical vapor infiltration and the thickness was controlled via the infiltration time. Structural annealing of the PyC coated AMWCNT (AMWCNT/C) sheets at 2150 oC provided different results for different thickness coatings. Transmission electron microscopy images showed that the carbon deposited from acetylene formed laminar PyC coatings, resembling rough tube walls, on the CNT surfaces. Following the high temperature heat treatment, coatings from short PyC deposition times changed their structure, resulting in radial growth of the MWCNTs. Raman and X-ray diffraction measurements also revealed that the radially grown MWCNTs had graphitic quality very close to pristine nanotubes after annealing. Electrical conductivity of AMWCNT/C sheets after high temperature heat treatment was twice that of pristine AMWCNT sheets. The focus of this study was to determine the PyC coating thickness at which a rough PyC coating would no longer change it structure into new CNT walls. The samples treated longer than 30 minutes had much more disordered PyC deposited on the surface and the additional material did not form additional tube walls after thermal annealing. Read the full paper here.