Against the backdrop of the increasing energy crisis and environmental pollution, the exploration of low-cost, green, and sustainable energy sources has become more and more imperative. The rapid development of green energy has also stimulated the demand on energy storage and conversion systems. Carbon-based aerogels (CAs), as emerging electrode materials and characterized by sustainable and high performance, have attracted significant attentions. The present review provides a comprehensive overview of the fabrication of CAs, and especially focuses on the recent advances in optimizing the electrochemical performance of CAs for applications in supercapacitors, batteries, and electrocatalysis from the perspectives of the structural design, conductivity enhancement, and chemical modifications. Critical discussion and analyses are conducted on the surface/interface properties of CAs as electrodes and catalytic material, as well as their advantages and disadvantages of advanced synthesis strategies. Discussion is also expanded on key challenges, current issues, and the prospects for their laboratory and industrial applications. This work offers valuable insights into the rational structural design and functionalization of CAs and is expected to serve as a foundation for the commercial development of electrode materials in energy storage and conversion devices.The present review provides an overview of recent advances in optimizing the electrochemical properties of carbon based aerogels for energy storage and energy conversion.The surface/interface properties, structural design and synthesis strategies used as electrode and catalysis materials were discussed. Meanwhile, challenges and prospects of their applications were also proposed.