The macroscopic coaxial carbon cylinders (dia. ∼ 0.5 cm with varying lengths, ∼ 7–10 cm) consisting of aligned carbon nanotube (CNT) stacks have been prepared by controlled spray pyrolysis method. The coaxial carbon cylinders of CNT stacks have been formed directly inside the quartz tube. Another study is done on multi-walled CNTs (MWNTs)–polymer (e.g. polyethylene oxide (PEO), polyacrylamide (PAM)) composite films. We have investigated the structural, electrical and mechanical properties of MWNTs–PEO composites. Composites with different wt% (between 0 and 50 wt% of MWNTs) have been prepared and characterized by the scanning electron microscopic technique. Enhanced electrical conductivity and mechanical strength were observed for the MWNTs–PEO composites. We have also studied the electrical property of MWNTs–PAM composite films.