Mechanically interlocked molecules (MIMs), such as bistable catenanes and bistable rotaxanes, have been used to bring about actuation in nanoelectromechanical systems and molecular electronic devices. The elaboration of the structural features of MIMs into polymers and metal-organic frameworks (MOFs) might allow the utilization of molecular motion to impact the bulk properties of the solid-state materials. This dissertation describes successful attempts in realizing such concept. First of all, polymers which contain π-electron-donating 1,5-dioxynaphthalene (DNP) units encircled by cyclobis-(paraquat- p-phenylene) (CBPQT⁴⁺), a π electron-accepting tetracationic cyclophane, synthesized by using the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) was reported. These poly[n]rotaxanes adopt a well-defined "folded" secondary structure by virtue of the judicious design of two DNP-containing monomers with different binding affinities for CBPQT⁴⁺. Secondly, obtained by a similar approach, a poly[ n]rotaxane containing alternating DNP and tetrathiofulvalene (TTF) units encircled by CBPQT⁴⁺ rings was studied, which shows reversible bistability controlled by electrochemical redox processes. The poly[ n]rotaxane was incorporated into solid-state devices by means of spin-coating, which exhibit switching behavior depending on electrode choices. In order to extend the exploration to the area of MOFs, rigid organic dicarboxylic acids containing crown ethers were synthesized. These novel compounds retain the characteristics of their parent crown ethers since they can bind cationic guests and serve as templates for making MIMs. The binding behavior of BPP34C10DA with the paraquat dication (PQT²⁺) has been investigated, and the BPP34C10DA-based [2]catenane (H₂BPP34C10DC-CAT) were prepared. The former was used to synthesize MOF-1001, which adopts the primitive cubic structure and is capable of docking PQT²⁺ guests within the macrocycles in a stereoelectronically controlled fashion. The latter was used to construct MOF-1011, whose two-dimensional layered structure contains [2]catenanes in an extremely dense and highly ordered fashion. These studies not only represent efficient approaches to the preparation of polymers and metal-organic frameworks with previously undescribed functionalities, but also set the stage for the development of next-generation solid-state materials with unprecedented complex functions.