This work reports for the first time the synthesis of γ-(Al1-xFex)2O3 solid solutions with a high specific surface area (200-230 m2/g) by the decomposition of metal oxinate [(Al1-xFex)(C9H6ON)3] and investigated the potential of these materials as catalysts for the synthesis of carbon nanotubes by catalytic chemical vapor deposition using methane or ethylene as carbon the source. The nanocomposite powders prepared by reduction in H2-CH4 contain carbon nanotubes (CNTs), which are mostly double-walled but also contain a fair amount of undesirable carbon nanofibers, hollow carbon particles, and metal particles covered by carbon layers. Moreover, abundant metallic particles are observed to cover the surfaces of the matrix grains. By contrast, the nanocomposite powders prepared by reduction in N2-C2H4 are not fully reduced, and the CNTs are much more abundant and homogeneous. However, they are multiwalled CNTs with a significant proportion of defects. The powders were studied by several techniques including Mössbauer spectroscopy and electron microscopy.