Iron-oxide nanoparticle monolayers and multilayers were assembled using dc electrophoretic deposition. The rate of deposition and the total particle deposition were controlled by varying the concentration of nanoparticles and the deposition time, respectively. Using scanning electron microscopy, we performed a time-resolved study that demonstrated the growth of the monolayer from a single isolated nanoparticle to a nearly complete layer. We observed tight, hexagonal packing of the nanoparticles indicating strong particle-particle interaction. Multilayer growth was assessed using scanning electron microscopy and atomic force microscopy, revealing a monolayer-by-monolayer growth process.