Abstract The cytoskeleton is one of the most important cellular components. Up to now, most of the reported artificial cytoskeletons are based on a gel‐in‐vesicle strategy. Herein, we report a membrane‐bound inward‐growth pathway to prepare cytoskeleton‐like and radially aligned nanofibers grown from capsule membranes to get membrane‐bound artificial cytoskeletons (MACs). The mechanism therein is disclosed through the direct observation of the intermediates in both dried and liquid states. Furthermore, the as‐prepared MACs show a selective disassembly behavior in the presence of reductants: both capsule membranes and MACs can be disassembled or only MACs can be disassembled through the selective introduction of dynamic disulfide bonds (DS) into them and by the switch of ultraviolet (UV) irradiation. The present work provides a new hierarchical self‐assembly way to construct artificial cytoskeletons with controlled compositions and orientations.
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