In response to the increasing demand for flexible and portable electronics, there is a growing need for next generation energy storage devices that can deliver both high power density and long-term durability. To effectively support such applications, these systems should exhibit exceptional electrochemical performance, as well as operational stability under a wide range of mechanical and environmental stresses. Macromolecules with high thermal stability and thermo-oxidative stability complemented by excellent solvent resistance, good electrical and mechanical properties and chemical resistance make them as great candidates as electrode materials. This talk covers our recent works on macromolecular electrode materials for energy storage devices. Our studies not only elucidate the critical role of molecular functionalization in modulating the interfacial chemistry and electrochemical behavior of carbon-based electrodes but also provide a rational and scalable design strategy for high performance energy storage devices via precise molecular engineering of macromolecular building blocks.