Three‐Dimensional Graphene Aerogel Materials for Supercapacitors: Strategies and Mechanisms

Graphene aerogels (GAs) exhibit exceptional potential in energy storage, particularly for high‐capacity supercapacitors (SCs), owing to their unique three‐dimensional (3D) porous structure, high conductivity, and mechanical stability. Despite limitations in electron transport and surface polarity, their performance can be enhanced through structural optimization and synthesis strategies. This review traces the evolution of GAs from 1931 to 2024, integrating historical development with recent breakthroughs. It analyzes the synergistic effects of synthesis methods (self‐assembly, template‐assisted) and drying techniques (freezing/supercritical/ambient‐pressure drying), elucidating structure–performance relationships and electrochemical mechanisms. This review also details the current research status of GAs applied in double‐layer capacitors and pseudocapacitors. It identifies existing issues and summarizes ways to improve performance. Additionally, the research prospects of AI‐assisted and in situ dynamic characterization in the development of GAs are outlined. In conclusion, this review aims to further advance high‐performance GA electrode materials for SC applications and to anticipate future technological trends, providing a basis and academic reference for researchers in the energy storage field.