Aggregation and coalescence are major drawbacks that contribute to polydispersity in microparticles and nanoparticles fabricated from diverse biopolymers. This study presents the evaluation of a novel method for the direct, electrospray-induced fabrication of small, CaCl 2 /ethanol-hardened low methoxy pectin/arabinoxylans composite microbeads. The electrospray method was evaluated to control particle size by adjusting voltage, flux, and crosslinking solution content of CaCl 2 /ethanol. A bead diameter of 1µm was set as reference to test the capability of this method. Insulin was chosen as a model carried molecule. Statistical analysis was a central composite rotatable design (CCRD) with a factorial arrangement of 2 4 . The variables studied were magnitude and particle size dispersion. For the determination of these variables, light diffraction techniques, scanning electron microscopy, transmission electron microscopy, and confocal laser scanning microscopy were used. Major interaction was found for ethanol and CaCl 2 as well as flow and voltage. Stable spherical structures of core-shell beads were obtained with neither aggregation nor coalescence for all treatments where ethanol was included in the crosslinking solution, and the average diameter within 1 ± 0.024 µm for 11 KV, 75% ethanol with 11% CaCl 2 , and flow of 0.97 mL/h.