LAUSR

Significance Molecular self-assembly provides a bottom-up platform to design supramolecular functional materials, attracting numerous interests in material sciences. The utilization of platinum(II) complexes as building blocks of supramolecular assemblies opens up the unique noncovalent Pt···Pt interaction as one of the driving forces, imparting the supramolecular materials with rich spectroscopic features. However, the exact role of Pt···Pt interactions in molecular assembly remains elusive. The current study combines experimental and computational techniques to elucidate the role of Pt···Pt interactions in the self-assembly process of a representative amphiphilic platinum(II) complex. This work demonstrates the directional role of Pt···Pt interactions in assisting the molecular assembly in an anisotropic manner, achieving the formation of ordered self-assembled structures.