<p>As organo-electrocatalysts garner increasing attention from both the inorganic and organic chemistry domains, it becomes necessary to develop a comprehensive database of effective catalysts for diverse anodic and cathodic reactions, which are pivotal for sustainable human development. The obstacles impeding the application of organo-electrocatalysts can be classified into three primary categories: the ambiguous nature of the interactions between the electrode and organic molecules, inadequate efficiency in synthesizing high-value chemicals, and suboptimal durability under commercial production conditions. One potential resolution to overcome these challenges relies on molecular catalysts, owing to their structural diversity, controllable synthesis and well-established mechanistic understanding. Here we propose a class of organo-electrocatalysts with amide groups to facilitate electrode oxidation and reduction processes. These catalysts exhibit high activity (overpotential of 91 mV@1 A cm⁻²), high selectivity (99.9%) and high durability (1 A cm⁻² for 200 h) towards the inorganic chlorine evolution reaction under industrial conditions (5 M NaCl, pH 2, 90 °C). In addition, these catalysts also demonstrate robust activity across various chlorine-related organic reactions. Therefore, this work holds promise for the design of molecular catalysts applicable to both inorganic and organic synthesis.</p><p></p>