The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10. 1002/smll.201803858. Graphene is widely applied as an electrode material in energy storage fields. However, the strong π-π interaction between graphene layers and the stacking issues lead to a great loss of electrochemically active surface area, damaging the performance of graphene electrodes. Developing 3D graphene architectures that are constructed of graphene sheet subunits is an effective strategy to solve this problem. The graphene architectures can be directly utilized as binder-free electrodes for energy storage devices. Furthermore, they can be used as a matrix to support active materials and further improve their electrochemical performance. Here, recent advances in synthesizing 3D graphene architectures and their composites as well as their application in different energy storage devices, including various battery systems and supercapacitors are reviewed. In addition, their challenges for application at the current stage are discussed and future development prospects are indicated. Energy Storage www.small-journal.com electrochemically active sites; [14] and iv) combining conductive polymer with 3DGAs to effectively suppress the shuttle effect in lithium-sulfur (Li-S) batteries, increase the specific capacity of supercapacitors, etc. [15] The functionalized 3DGAs combined with the electrochemically active materials could integrate the benefits of each component, thereby improving the specific performance in corresponding applications.In this paper, we first summarized the recent advances in the construction strategies for 3DGAs. Then, we reviewed the applications of 3DGAs and 3DGA-based composite materials in various energy storage devices, including i) lithiumion batteries (LIBs) and sodium-ion batteries (SIBs); ii) Li-S batteries; iii) lithium metal batteries; iv) other battery systems like Li-O 2 batteries; and v) electrochemical supercapacitors. By making systemically summary and comparison, we concluded the achievement and challenges of 3DGAs and their composites in these areas, and the likely future developments are also discussed.