Different techniques are being developed for fabricating microcapsules; it is still a challenge to fabricate them in an efficient and environment‐friendly process. Here, a one‐step green route to synthesize silk protein sericin‐based microcapsules without any assistance of organic solvents is reported. By carefully changing the concentration of calcium ions accompanied with stirring, the morphology of the microcapsules can easily be regulated to form either discoidal, biconcave, cocoon‐like, or tubular structures. The chelation of Ca2+ and shearing force from agitation may induce the conformational transformation of sericin, which possibly results in the formation of microcapsules through the self‐assembly of the protein subsequently. The as‐prepared cocoon‐like microcapsules exhibit pH‐dependent stability. A potential application of microcapsules being fabricated from natural water‐soluble silk protein sericin for controlled bioactive molecules loading and release system by a pH‐triggered manner is quite feasible.
