Mechanically interlocked polymers (MIPs) derive their name from their unique mechanical bonding motif in which the polymer components are constrained in space but not physically bound to each other. MIPs have received increasing attention of late due to their potential in the fields of molecular machines and smart soft materials. Of these materials, one of the most synthetically challenging architectures is the poly[n]catenane, a polymer composed only of interlocking macrocyclic rings, where n is equal to the number of interlocked rings. The interlocking macrocycles allow the polymer to display different motions than those seen in a traditionally covalently bound material, suggesting that the poly[n]catenane may display uncommon dynamics in solution and unique material properties, such as superior strength and flexibility. In 2017, the first poly[n]catenane synthesis was reported, created from a metallosupramolecular polymer (MSP) template consisting of alternating units of macrocyclic and linear thread-like monomers. Ring closure of the thread components yielded the interlocked polymer and this initial report focused primarily proving the existence of the poly[n]catenane structure, while including basic characterization of polymer architecture. This dissertation represents the continuation of that work. Firstly, the original synthetic process was explored in depth, with a focus on the MSP precursor. This study primarily probed the effects of the reaction concentration on the overall yields and product mixtures of the poly[n]catenane. Secondly, a new series of linear thread-like monomers was developed to test the applicability of this method beyond the initial synthesis and determine how the structure of this component changes the final architecture of the poly[n]catenane. Thirdly, a library of new macrocyclic monomers was created to test the effects of both size and rigidity of these components on the overall poly[n]catenane synthesis and the formation of unwanted byproducts. Fourth and lastly, steps toward creating more complex poly[n]catenane co-polymers and networks have been taken.