AbstractA solvent driven molecular shuttle that contains a TCBD chromophore and in which the macrocycle can be positioned close to or far from the TCBD unit with a change of solvent is prepared. Several distinct nanostructures are obtained by control of the shuttling movement of the macrocycle: i) in a mixed solvent of CHCl3/n‐C6H14 (1/1, v/v), the macrocycle locates at the peptide station, and interlaced nanofibers form as a result of the extended intermolecular dipole–dipole interactions of the TCBD units; ii) in a solvent of dimethyl sulfoxide, the macrocycle moves along the long alkyl‐chain, and worm‐like nanoparticles form because the macrocycle obstructs the intermolecular dipole–dipole interactions of the TCBD units. This system confirms that the molecular aggregation behaviors can be controlled by the shuttling movement of the macrocycle. Exploitation of the molecular shuttle to control the molecular aggregation behaviors will provide greater understanding in the field of molecular shuttle applications.