Micro-supercapacitors (MSCs) are a class of energy storage devices that stand out for their high power density, long cycle life, and environmental friendliness. The key to improving their electrochemical performance lies in selecting appropriate electrode materials. This review highlights the latest research achievements, challenges, opportunities, and perspectives in the field of electrode materials for MSCs. It covers the working principles, structural classifications, and physiochemical and electrochemical characterization techniques of MSCs. Various materials and preparation methods are discussed, emphasizing the relationship between MSC performance and the structure and composition of electrode materials. The review also provides suggestions for accelerating the development of electrode materials to facilitate the commercialization of MSCs. Key topics include carbon-based materials, metal compounds, conductive polymers, coordination polymers, porous polymers, and composite electrodes. The review concludes with a discussion on future development and existing problems in the field.Micro-supercapacitors (MSCs) are a class of energy storage devices that stand out for their high power density, long cycle life, and environmental friendliness. The key to improving their electrochemical performance lies in selecting appropriate electrode materials. This review highlights the latest research achievements, challenges, opportunities, and perspectives in the field of electrode materials for MSCs. It covers the working principles, structural classifications, and physiochemical and electrochemical characterization techniques of MSCs. Various materials and preparation methods are discussed, emphasizing the relationship between MSC performance and the structure and composition of electrode materials. The review also provides suggestions for accelerating the development of electrode materials to facilitate the commercialization of MSCs. Key topics include carbon-based materials, metal compounds, conductive polymers, coordination polymers, porous polymers, and composite electrodes. The review concludes with a discussion on future development and existing problems in the field.