Multi-layer ultrathin polymer films have been deposited on the surfaces of nanoparticles of alumina using a plasma polymerization treatment. The nanoparticles ranged from 10-150 nm in spherical shapes. High-resolution transmission electron microscopy (HRTEM) experiments showed that an extremely thin film of the pyrrole layer (10-20 Å) was uniformly deposited on the surfaces of the nanoparticles. In particular, the particles of all sizes (10-150 nm) exhibited equally uniform ultrathin films indicating well-dispersed nanoparticles in the fluidized bed during the plasma treatment. After single layer coating, hexamethyldisiloxane (HMDSO) was coated again as a second layer onto the surface of pyrrole. Subsequently, a third layer of pyrrole was coated on the top of HMDSO film completing the multi-layer coating process. Time-of-Flight Secondary ion mass spectroscopy (TOFSIMS) experiments confirmed the deposition of these multi-layer thin films on the nanoparticles. The deposition mechanisms and the effects of plasma treatment parameters are discussed.