Supramolecular assemblies with diverse morphologies are crucial in determining their biochemical or physical properties. However, the topological evolution and self‐assembly intermediates as well as the mechanism remain elusive. Herein, a dynamic morphological evolution from solid nanospheres to superhelical nanofibers is revealed via self‐assembly of a minimal l‐tryptophan‐based derivative (LPWM) with various mixed solvent combinations, including the formation of solid nanospheres, the fusion of nanospheres into pearling necklace, the disintegration of necklace into short nanofibers, the distortion of nanofibers into nanotwists, and the entanglement of nanotwists into superhelices. It is found that the breakage of intramolecular H‐bonds and reconstruction of intermolecular H‐bonds, as well as the variation of aromatic interactions and hydrophobic effects, are the key driving forces for topological transformation, especially the dimensional evolution. The nanospheres and nanofibers demonstrate discrepant behaviors towards mouse neural stem cell (NSC) differentiation that compared with negligible impact of nanospheres scaffold, the nanofibers scaffold is favorable for NSC differentiation into neurons. The remarkable dynamic regulation of assembly process, together with the NSC differentiation on twisted nanofibers are making this system an ideal model to interpret complex proteins fibrillation processes and investigate the structure–function relationship.

中文翻译：

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从纳米球到超螺旋的溶剂控制拓扑演化

具有多种形态的超分子组装对于确定其生物化学或物理性质至关重要。但是，拓扑演化和自组装中间体以及该机制仍然难以捉摸。这里，从固体纳米球以超螺旋纳米纤维的动态形态演变经由自组装的最小的揭示升基于色氨酸的衍生物（LPWM），具有多种混合溶剂组合，包括形成固体纳米球，将纳米球融合成珍珠项链，将项链分解成短纳米纤维，将纳米纤维扭曲成纳米捻以及将纳米捻缠结成超螺旋。发现分子内氢键的断裂和分子间氢键的重建以及芳族相互作用和疏水作用的变化，是拓扑转换尤其是尺寸演变的关键驱动力。纳米球和纳米纤维对小鼠神经干细胞（NSC）的分化表现出不同的行为，与纳米球支架的影响微不足道相比，纳米纤维支架有利于NSC分化为神经元。