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A major challenge in tissue engineering is the formation of vasculature in tissue and organs. Recent studies have shown that positively charged microspheres promote vascularization, while also supporting the controlled release of bioactive molecules. This study investigated the development of gelatin-coated pectin microspheres for incorporation into a novel bioink. Electrospray was used to produce the microspheres. The process was optimized using Design-Expert® software. Microspheres underwent gelatin coating and EDC catalysis modifications. The results showed that the concentration of pectin solution impacted roundness and uniformity primarily, while flow rate affected size most significantly. The optimal gelatin concentration for microsphere coating was determined to be 0.75%, and gelatin coating led to a positively charged surface. When incorporated into bioink, the microspheres did not significantly alter viscosity, and they distributed evenly in bioink. These microspheres show great promise for incorporation into bioink for tissue engineering applications.