Binaphthyl-based systems have been under extensive investigation during the past years as sensors, host molecules, asymmetric catalysts, chiral-conjugated polymers, and high performance materials. This review mainly focuses on the synthesis, structural investigation, and applications of binaphthyl-based macromolecules. It begins with a brief overview on design and synthesis of direct or indirect-linked binaphthyl-based monomers. Fundamentals of the synthesis and macromolecular structure of binaphthyl hosts as chiral catalysts for various asymmetric organic reactions are then provided. In addition, recent complexation studies of some podands and macrocycles derived from binaphthyls are highlighted. Furthermore, the synthesis and properties of main chain chiral conjugated polymers having optically active 1,1′-binaphthyls are discussed. Finally, we focus on recent work involving the incorporation of binaphthyl units into the macromolecules backbone to prepare processable high performance polymers.