We describe the high yield synthesis of multi-walled carbon nanotubes (MWCNTs) and the determination of the optimum production conclitions. The method involves the catalytic pyrolysis of solid Ni(dMg)(2) under an At atmosphere. The obtained materials were characterized by scanning electron microscopy (SEM), energy dispersive X-ray (EDX) analysis, high resolution transmission electron microscopy (HRTEM), Xray diffraction (XRD), Raman spectroscopy and thermogravimetry analysis (TGA). The data revealed the formation of MWCNTs surrounded by a varying quantity of byproducts such as amorphous carbon and metallic particles, depending mainly on the reaction temperature. Pyrolysis of Ni(dMg)2 at 900 degrees C results in the production of nanotube material with the highest degree of crystallinity. (C) 2008 Elsevier Ltd. All rights reserved.