This paper presents a novel and facile approach to fabricate robust crystal balls directly through the self-assembly of soft colloidal polymer spheres by the aid of nano silica using an electrospraying technique. In this approach, soft colloidal polymer spheres are synthesized by emulsion polymerization and then blended with colloidal silica to obtain nanocomposite dispersion. When this dispersion is loaded into an injector and forced to flow through the nozzle under direct electric field, the detached droplets are collected by an oil solvent. As water and solvent evaporate, the colloidal polymer spheres and silica beads can directly self-assemble into robust crystal balls. Neither soft matrix nor post-treatment is needed. The obtained crystal balls have not only excellent mechanical properties to withstand external forces such as cutting, puckering, and bending, but also reversible deformation.