In this study, the technological feasibility of an electrospray-based flame synthesis process for the production of thin films of nanosized metal oxide particulates was investigated. On the basis of published results on electro-hydrodynamic atomization, a spray system was designed, implemented, and tested. Initial tests focused on synthesis of yttria-stabilized zirconia (YSZ) particulates, and the results showed that aggregates with quasi-monodisperse primary particle sizes below 100 nm with cubic-fluorite crystal phase composition can be manufactured through this production route. These tests utilized organometallic solutions of Zr-n-propoxide and Y-2-methoxyethoxide in a mixture of n-propanol and 2-methoxyethanol, which were electrosprayed into the postflame flow of a multielement diffusion burner. Both theoretical analysis and experimental evidence indicate that controlled synthesis of particulate with narrow particle size distribution is feasible. The radial arrangement of electrospray emitters chosen for the initial experiments appears to be a promising spray configuration for further development.