Fe3O4 Nanoparticles produce stable self-assembly film with cationic diazoresin (DR) on silicon surface, after reduction of Fe3O4 the multi-walled carbon nanotubes (MWNTs) were grown on the silicon substrate via chemical vapor deposition (CVD) method. The Fe3O4 nanoparticles capped with polyacrylic acid (PAA) can avoid the aggregation of the nanoparticles effectively as well as improving the efficiency of the self-assembly. As a result the thin films with evenly distributed Fe3O4 nanoparticles and the nanotubes uniformly distributed on Si substrate were obtained.