Here, we report the hierarchical self-assembly of a cationic gemini amphiphile, Azo 1, in a composition gradient solution generated using solvent evaporation. As the gradient solution is formed, Azo 1 forms nanorods in the lower region of the solution. Depending on solvent composition, these nanorods can further develop into nanofibres, which can then intertwine to form double helices and other types of nanohelices in the upper region of the solution. Finally, a macroscopic wire bundle is formed via the fusion of nanohelices; this ribbon-like bundle exhibits elasticity and linear ohmic resistance properties. More intriguingly, this bundle exhibits photoresponsive properties that affect its deformation and conductivity, as well as a rapid electroresponse that affects its conductivity, indicating that it is feasible to control the charge pathway.
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