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Spin crossover (SCO) is one of the most widely studied phenomena in transition metal complexes, in part due to the possible technological applications of such species in molecular electronics, memory storage, electrochromics, and display devices. Any transition metal complex with a d⁴–d⁷electron configuration, such as 2+ and 3+ ions of Cr, Mn, Fe, and Co, can theoretically exhibit SCO effects which depend highly on the coordination environment and ligand field strength. Redox-coupled SCO processes provide a mechanism to enhance the molecular bistability and trigger transitions between low- and high-spin states. Similar reaction mechanisms often occur in electrocatalytic and enzymatic reactions. The electrochemical response of redox-coupled SCO processes can be modeled as a square scheme containing two one-electron reactions and two chemical steps, resulting in a separation of anodic and cathodic waves. Herein we describe the influence of ligand coordination and structural changes on the redox-coupled SCO properties of several Co complexes. This structural-functional analysis allows us to understand the fundamental properties that control redox-coupled SCO processes and optimize redox bistability for a range of applications.