To assemble functional molecular units into a desired structure while controlling positional and orientational order is a key technology for the development of high-performance organic materials that exhibit electronic, optoelectronic, biological and even dynamic functions. For this purpose, we cannot rely simply on the inherent self-assembly properties of the target functional molecular units, since it is difficult to predict, based solely on the molecular structure, what structure will be achieved upon assembly. To address this issue, it would be useful to employ molecular building blocks with self-assembly structures that can be clearly predicted and defined, to make target molecular units assemble into a desired structure. To date, various motifs of molecular assemblies, polymers, discrete and/or three-dimensional metal-organic complexes, nanoparticles and metal/metal oxide substrates have been developed to create materials with particular structures and dimensionalities. In this perspective, we define such assembly motifs as "supramolecular scaffolds". The structure of supramolecular scaffolds can be classified in terms of dimensionality, and they range in size from nano- to macroscopic scales. Functional molecular units, when attached to supramolecular scaffolds either covalently or non-covalently, can be assembled into specific structures, thus enabling the exploration of new properties, which cannot be achieved with the target molecular units alone. Through the classification and overview of reported examples, we shed new light on supramolecular scaffolds for the rational design of organic and polymeric materials.