With the rapid development of mobile electronics and electric vehicles, the future development of supercapacitors focuses on not only high energy and power densities but also device minimization and lightweight. Although activated carbon based on an electric double-layer mechanism has been used in commercialized supercapacitors, it is unsatisfied with the ever-increasing demands for high energy and power device in a limited space. Therefore, it is urgent for the design and preparation of advanced carbon electrode materials with both high gravimetric and volumetric performance without sacrificing their inherent high-rate ability and long-lifespan. This review presents the latest developments in highefficiency utilization of carbon materials for supercapacitors including the carbon surface and space. We discuss the impact of pore engineering, conductive network, and surface engineering on the energy storage ability of the carbon materials, and highlight the synthesis and characterization as well as the relationship between their structural properties and electrochemical performance. Finally, future research towards developing advanced carbon supercapacitors, perspectives, and challenges are outlined.