Monolayer and multilayer ultrathin films comprised of nanosized iron oxide (Fe3O4) particles and polyimide molecules have been fabricated on single crystal silicon and quartz substrates by a novel layer-by-layer electrostatic self-assembly process. This process involves the alternate dipping of a substrate into an aqueous solution of anionic polyimide precursor (polyamic acid salt, PAATEA), followed by dipping into an aqueous solution of polycation polydiallyldimethylammonium chloride (PDDA) which coats on nanoscale Fe3O4 particles as a stabilizer. The growth process and the structure have been characterized using UV-vis spectroscopy, contact angle, and ellipsometry measurements. The results suggest that well-ordered uniform monolayer and multilayer magnetic films have been formed on silicon and silica surfaces. A recently developed highly sensitive fiber optic magnetic field sensor was used to probe the small magnetic field intensity produced by the multilayer films. (C) 1997 American Institute of Physics.