Three-dimensional organized unidirectionally aligned and responsive supramolecular structures have much potential in adaptive materials ranging from biomedical components to soft actuator systems. However, to control the supramolecular structure of these stimuli responsive, for example photoactive, materials and control their actuation remains a major challenge. Toward the design of “artificial muscles”, herein, we demonstrate an approach that allows hierarchical control of the supramolecular structure, and as a consequence its photoactuation function, by electrostatic interaction between motor amphiphiles (MA) and counterions. Detailed insight into the effect of various ions on structural parameters for self-assembly from nano- to micromet...