The control of the morphology of nanostructured particles prepared by the spray drying of nanoparticle sol was investigated experimentally and the results are qualitatively explained based on available theory. A theoretical analysis indicates that the structural stability of the droplet and the hydrodynamic effects during the drying process play important roles in controlling the morphology of the resulting particles. The size of the sol in the droplet, droplet size, viscosity of droplet, drying temperature, gas flow rate, and addition of surfactant are all crucial parameters that affect the morphology of particles. Experimentally, nanostructured silica particles were prepared from a nanosize silica sol under various preparation conditions. Doughnut-shaped particles can be produced when the droplet size is large, in conjunction with high temperature, high gas flow rate and in the presence of an added surfactant. Appropriate choice of the spray drying method permits control of the particle size and shape, ranging from spheres to ellipsoids as well as doughnut-shaped particles by varying the preparation conditions. The results open a new route to controlling the formation of a wide variety of nanostructured particles.