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, e.g., photoactive materials and control their actuation remains a major challenge. Towards 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 counter ions. Detailed insight into the effect of various ions on structural parameters for self-assembly from nano- to micro-meter scale in water including nanofiber formation and nanofiber aggregation as well as the packing structure, degree of alignment and actuation speed of the macroscopic MA strings prepared from various metal chlorides solution, as determined by electronic microscopy (SEM), X-ray diffraction (SAXS), and actuation speed measurements, is presented. Macroscopic MA strings prepared from calcium and magnesium ions provide a high degree of alignment and fast response photoactuation. By the selection of metal ions and chain length of MAs, the macroscopic MA string structure and function can be controlled demonstrating the potential of generating multiple photoresponsive supramolecular systems from an identical molecular structure.