Oxidized corn starch-gelatin (OCS-Gel) was successfully synthesized by the electrochemical-assisted oxidation method. The introduction of spray-drying technology, as an advanced method for the postprocessing of sample solution, also has greatly improved the application property of blend. The corn starch was gelatinized first, and then mixed with gelatin solution to prepare the blend solution in the electrolyzer with current (120 mA) and 0.5% sodium chloride. Finally, the prepared OCS-Gel solution was dehydrated and granulated using the spray-drying process to obtain the powder particles of OCS-Gel. The spray-dried OCS-Gel was characterized by FT-IR, XRD and SEM. The introduction of active groups (amino, carboxyl, carbonyl) promoted OCS-Gel hydration and swelling. In addition, compared with CS the crystallinity of spray-dried OCS-Gel decreased obviously. The OCS-Gel formed a hollow or deflated spherical structure. The electrochemical-assisted oxidation and spray-drying technology were masterfully combined to prepare the OCS-Gel, which can dramatically improve the application performance of biomaterials.