Al1.8Fe0.2O3 amorphous solid solution have been calcified at temperatures between 1025 and 1100 degrees C and the obtained powders have been reduced in a H-2-CH4 gas mixture (12 mol% CH4) at 1050 degrees C in order to prepare carbon nanotubes (C-NTs)-Fe/Fe3C-Al2O3 nanocomposite powders. The calcination at 1100 degrees C leads to powders containing an alpha-Al2-2xFe2xO3 solid solution (x < 0.1) and some traces of a Fe-rich phase (alpha-Fe2-2yAl2yO3) that gives, under reduction, large Fe particles which catalyze the growth of ribbon like filaments. An alpha-Al1.8Fe0.2O3 monophased solid solution with a higher specific surface al ea is obtained after a calcination at only 1050 or 1025 degrees C. In the corresponding composite powders, all filaments are isolated C-NTs or bundles of C-NTs and the high specific area is beneficial to both the quantity and the quality parameters which are greatly enhanced in comparison with previous results. About 20% of the observed C-NTs are single wall nanotubes (SWNTs). The majority of the observed multiwall nanotubes (MWNTs) have only two walls and the inner diameters are distributed between 0.8 and 6 nm, with a peak at 2 nm. The in-situ catalysis by selective reduction of a solid solution allows for production of nanocomposite powders containing very large quantities of high quality C-NTs.