The alignment of multiwalled carbon nanotubes (MWNTs) has been accomplished through deposition ofuniform layers of magnetite/maghemite nanoparticles (diameter = 6-10 nm) and use of an external magneticfield. The coating of CNTs with magnetic nanoparticles was performed by combining the polymer wrappingand layer-by-layer (LbL) assembly techniques. The particle-coated MWNTs are superparamagnetic and canbe aligned at room temperature on any substrate by deposition from an aqueous solution in an external fieldB = 0.2 T. The volume magnetization of the particle coated MWNTs is found to be enhanced by 17%compared to the pure particles in a powder indicating that either the adsorption process onto the CNTs changesthe particle magnetization, or the MWNTs carry an intrinsic magnetization due to remaining Ni used as acatalyst for the growth process.