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The microsphere building blocks with controlled diameter are prepared from the naturally occurring biopolymer, silk fibroin, and then act as stabilizers for oil\u2010in\u2010water (O\/W) emulsion and organized themselves on the surface of chloroform droplets to form the capsules. The concentration of the protein\u2010based microspheres and the binding polycacrolactone is used to tailor the size, as well as the permeability of the resultant capsules. Furthermore, microencapsulation of fluorescently labeled macromolecules (20\u20132000 KDa) is demonstrated. The permeability of the capsules is observed to be stimuli responsive, making it possible to incorporate a pH\u2010triggered payload release from the capsules. 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