| Summary: | Abstract Multicompartmental microparticles (MCMs) have attracted considerable attention in biomedical engineering and materials sciences, as they can carry multiple materials in the separated phases of a single particle. However, the robust fabrication of monodisperse, highly compartmental MCMs at the micro‐ and nanoscales remains challenging. Here, a simple one‐step and oil‐free process, based on the gas‐flow‐assisted formation of microdroplets (“gas‐shearing”), is established for the scalable production of monodisperse MCMs. By changing the configuration of the needle system and gas flow in the spray ejector device, the oil‐free gas‐shearing process easily allows the design of microparticles consisting of two, four, six, and even eight compartments with a precise control over the properties of each compartment. As oils and surfactants are not used, the gas‐shearing method is highly cytocompatible. The versatile applications of such MCMs are demonstrated by producing a magnetic microrobot and a biocompatible carrier for the coculturing of cells. This research suggests that the oil‐free gas‐shearing strategy is a reliable, scalable, and biofriendly process for producing MCMs that may become attractive materials for biomedical applications.
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