Exploiting Coordination Isomerism for Controlled Self‐Assembly

We exploited the inherent geometrical isomerism of a Pt(II) complex as a new tool to control supramolecular assembly processes. UV irradiation and careful selection of solvent, temperature, and concentration leads to tunable coordination isomerism, which in turn allows fully reversible switching between two distinct aggregate species (1D fibers↔2D lamellae) with different photoresponsive behavior. Our findings not only broaden the scope of coordination isomerism, but also open up exciting possibilities for the development of novel stimuli‐responsive nanomaterials.