Metal–organic frameworks (MOFs) are crystalline, porous extended solids that are formed through coordination between metal cations and bridging organic ligands. Since their discovery in the late 1990s, MOFs have been a topic of acute interest in the scientific community due to their intrinsic porosity, high surface area, and precise tunability. However, MOFs are typically insulating, which limits the scope of their applications. The recent development of electrically conductive MOFs has opened the door to exciting multifunctional applications in electrocatalysis, advanced electrochemical energy storage, chemical sensing, and much more. However, a molecular-level understanding of charge transport in MOFs remains lacking. My research aims to address this knowledge gap through the investigation of one-dimensional (1D) metal organic chains. These 1D chains can be thought of as the primary subunit of higher-dimensional MOFs; they allow for high synthetic and electronic tunability, making them ideal model materials for studying the genesis and tuning of electronic properties in conductive MOFs. Here, I will present the synthesis of a series of highly-tunable 1D metal–organic chains that exhibit delocalized π systems and high electrical conductivity along with our studies of how structural parameters such as metal identity, chain structure (linear vs. zig-zag), and metal/ligand oxidation state can influence the overall electrical and magnetic properties of the resulting chain.