Structure elucidation of compounds is vital to understanding their chemical properties and reactivity. Nuclear Magnetic Resonance (NMR) spectroscopy plays a significant role in determining the structure of organic, inorganic, and biologically relevant compounds by using the magnetic properties of atomic nuclei to gather information about the physical and chemical properties of substances. Although instrumental advancements have allowed for structural elucidation of molecules as large as proteins and study of various nuclei such as 1H, 13C, 19F, 31P, and 29Si, minimal information exists on the use of isotopically-labelled nuclei to aid in structural determination of inorganic complexes. Thus, important information such as chemical shifts and coupling constants are absent from the literature. The use of asymmetric tetradentate ligands can impart unique electronic environments for trans-positioned isotopically-labelled ligands (13CN- and S13CN-) in octahedral compounds, allowing for spin-spin coupling through the metal center. Reactions with asymmetric Co(III) and Zn(II) complexes bearing isotopically labeled ligands were carried out and the products of these syntheses were analyzed using 13C NMR spectroscopy to investigate through metal carbon spin-spin coupling. The ligand frames were chosen based on their ability to position the isotopically labeled ligands trans- in the coordination sphere. Insight from this work may provide relevant information for structural determination of inorganic compounds.