Fully triggering the deep-seated potential of traditional nanomaterials, such as the classic spinel family, is of paramount importance in the field of materials science, which is yet believed to heavily depend on advanced conceptual designs and synthetic strategies. Herein, a type of inorganic-organic hybrid spinel oxide is designed using a π-conjugated azobenzene single-tooth coordination method to overcome their stubborn problems of moderate activity and phase instability in electrocatalytic reactions. Taking spinel Co