We describe a novel, facile method for the alignment of multi-walled carbon nanotubes (MWNTs) in a magnetic field facilitated by the decoration of the MWNTs with monodisperse γ-Fe2O3 magnetic (maghemite) nanoparticles. The tethering of the nanoparticles was achieved by the attachment of γ-Fe2O3 nanoparticles that were synthesized using a modified sol-gel process, onto the carboxylate-activated MWNTs. Sodium dodecylbenzene sulfonate (NaDDBS) was used to prevent the formation of an iron oxide 3D network. Various characterization methods were employed to confirm the formation of homogeneously-distributed and nearly-monodispersed iron oxide nanoparticles, and show that they were indeed tethered to the walls of the MWNTs. The γ-Fe2O3 nanoparticles imparted magnetic characteristics to the MWNTs, which in turn, were oriented parallel to the direction of an externally-applied magnetic field. This facile alignment of MWNT could promote the enhancement of various properties, e.g. mechanical and electrical properties, of the resulting composites. Moreover, this facile alignment at low magnetic fields, made possible by the magnetization of the carbon nanotubes through the tethering of maghemite nanoparticles, may be applied to a variety of other useful nanofillers, such a glass fibers, clay nanoparticles and cellulose nanowhiskers.