Vanadium redox flow battery (VRFB) is a type of energy storage device known for its large‐scale capacity, long‐term durability, and high‐level safety. It serves as an effective solution to address the instability and intermittency of renewable energy sources. Carbon‐based materials are widely used as VRFB electrodes due to cost‐effectiveness and well‐stability. However, pristine electrodes need proper modification to overcome original poor hydrophilicity and fewer reaction active sites. Adjusting the carbon structure is recognized as a viable method to boost the electrochemical activity of electrodes. This review delves into the advancements in research related to ordered and disordered carbon structure electrodes including the adjusting methods, structural characteristics, and catalytic properties. Ordered carbon structures are categorized into nanoscale and macroscale orderliness based on size, leading to improved conductivity and overall performance of the electrode. Disordered carbon structures encompass methods such as doping atoms, grafting functional groups, and creating engineered holes to enhance active sites and hydrophilicity. Based on the current research findings on carbon electrode structures, this work puts forth some promising prospects for future feasibility.