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The method uses a microfluidic device that contains a water-oil-water interface. The polymer complex is formed at the outermost water-oil interface, and the material to be encapsulated is introduced at the innermost water layer. Oppositely charged polymers are sequentially deposited onto a sacrificial solid core to form polyelectrolyte complex-based coatings on the solid particle. The core particle is removed via dissolution to form a hollow microcapsule, with target encapsulants introduced through the microcapsule shell by tuning the permeability to achieve microencapsulation.