Pyrene‐4,5,9,10‐tetraone (PTO), a coal tar derivative with redox‐active ortho‐carbonyl groups, has been intensively explored for sustainable organic electrodes due to its remarkably high capacity, superior redox robustness, and versatile cation storage. However, PTO often suffers from poor cycling stability due to its being soluble in organic electrolytes, which results in a detrimental shuttle effect and self‐discharge behavior. Its low electrical conductivity also results in poor rate performance, limiting practical applications. Therefore, different strategies have recently been developed to inhibit the solubility of PTO. In this review, the latest progress in enhancing the performance of PTO‐based electrodes and their applications in various battery types is presented. Firstly, a brief discussion on the relationship between the structural characteristics of PTO and its electrochemical performance is provided. Then, approaches to inhibiting the shuttle effect of molecular PTO are outlined and compared. Furthermore, the design and synthesis of PTO‐based polymer electrode materials are discussed. Finally, some perspectives and challenges are put forward regarding the performance improvement of PTO‐based electrode materials, inspiring further development of not only PTO but also other organic electrode materials in electrochemical energy storage applications.