Concepts from supramolecular chemistry have been introduced into polymer chemistry, generating supramolecular polymer chemistry. Supramolecular polymers have already been established as a new class of polymers capable of exhibiting unique functions, for example, stimulus-responsive, self-healing, analyte-sensing, and shape-memory features. Structural variations in supramolecular polymers are increased via the use of various supramolecular motifs. One of the recent focuses in supramolecular polymers is to control the chain structures of supramolecular polymers using various supramolecular structures. This chapter focuses in particular on supramolecular polymers with unique and controlled chain structures, which is organized by the preprogrammed supramolecular interactions. A brief historical overview is articulated in the introduction section. In the following sections, overview of early work on synthetic efforts related to supramolecular polymers and recent updates on the construction of unique and controlled chain structures for supramolecular polymers are provided. Finally, a summary of this chapter and potential challenges for the supramolecular polymers as functional materials are described.