This article presents the development of an on-line measurement and control system for process characterization and optimization of the nanoparticle manufacturing process, called the submerged arc-spray nanoparticle synthesis system (SANSS). To achieve optimized control of particle uniformity, this research investigates the feasibility of employing optical fiber probe and the dynamic light scattering (DLS) technique to monitor and control particle sizes. According to the theory of DLS, an on-line nanoparticle sampling and measurement system was developed and integrated with the SANSS as an important step to verify the measurement performance of the proposed method. To examine the measurement accuracy of the developed system, calibrated polystyrene latex particles with known accurate sizes were employed to verify the particle sizing accuracy of the proposed system. The data conformity between the measurement results of TiO, nanoparticles obtained by various methods, including TEM, a calibrated commercial particle sizing system and the on-line measurement system, has indicated that the developed method was feasible and effective.