The sophisticated hierarchical organization found in natural systems such as collagen is known to strongly dictate their physical properties and functions.1 Analogously, the properties of synthetic molecular systems have been shown to be highly dependent on the self-assembled structure formed at the nanometer length scale.2 However, understanding the intermolecularinteractions in an assembly at the molecular level and correlating them to the desired propertiesis a considerable challenge. We have taken a physical-organic chemist approach to understanding and harnessing non-covalent assemblies. In the first part of the talk, I will show our approaches to understand the non-covalent assembly mechanism of widely studied one-dimensional (1-D) synthetic supramolecular polymers at a molecular level in solution state.3 In addition to understanding the assembly in solution state, it is imperative to maintain the organization in the thin-film and solid- state for various applications. Hence, in the second part of the talk I will demonstrate our efforts towards controlling the chiral organization of both functional π-conjugated polymers and small molecules in the solid-state.