Graphitic carbon nitride with ordered two-dimensional structure displays multiple properties, including tunable structure, suitable bandgap, high stability, and facile synthesis. Many achievements on this material have been made in photocatalysis, but the advantages have not yet been fully explored in electrochemical fields. The bulk structure with low conductivity impedes charge-transfer kinetics during electrochemical processes. Excessive nitrogen content leads to insufficient charge transfer, while bulk structures produce tortuous channels for mass transport. Some attempts have been made to address these issues by nanostructure engineering, such as ultrathin structure design, heterogeneous composition, defect engineering, and morphology control. These structure-engineered nanomaterials have been successfully applied in electrochemical fields, including ionic actuators, flexible supercapacitors, lithium-ion batteries, and electrochemical sensors. Herein, a timely review on the latest advances in graphitic carbon nitride through various engineering strategies for electrochemical applications has been summarized. A perspective on critical challenges and future research directions is highlighted for graphitic carbon nitride in electrochemistry on the basis of existing research works and our experimental experience.